Propylene polymer compositions

ABSTRACT

A propylene polymer composition is prepared by mixing propylene homo- or co-polymer (A) obtained using a transition metal catalyst compound (h), defined herein, with a co-catalyst, e.g., organoaluminum oxy compound, with an olefin elastomer (D) and another olefin polymer (E), e.g., polyethylene. Alternatively, the combination of propylene polymer (A), olefin elastomer (D) and olefin polymer (E) is prepared by a multi-stage polymerization method. In both cases, the propylene homo- or co-polymer (A) may include a second propylene homo- or co-polymer (A′) wherein the ratio of intrinsic viscosities of propylene polymers (A) and (A′) is in the range of 3 to 30. These propylene polymer compositions are excellent in heat resistance, mechanical strength, tensile elongation at break, etc., and can be used in the fabrication of structural materials, films and sheets.

CROSS-REFERENCE TO RELATED APPLICATIONS

[0001] This application is a continuation of Ser. No. 09/966,652, filedNov. 10, 1997, which in turn is a continuation of application Ser. No.08/485,838, filed Jun. 7, 1995, abandoned, which in turn is a divisionof application Ser. No. 08/302,651, filed Sep. 8, 1994, now U.S. Pat.No. 6,156,844, which in turn was the National Phase entry under 35U.S.C. 371 of PCT/JP94/0002.4, filed Jan. 11, 1994.

FIELD OF THE INVENTION

[0002] The present invention relates to propylene polymer compositionseach comprising two kinds of propylene polymers and to propylene polymercompositions each comprising a propylene polymer and other olefin (co)polymer.

BACKGROUND OF THE INVENTION

[0003] Propylene polymers have been conventionally molded by variousmolding methods and the molded articles are applied to extensive uses.

[0004] The propylene polymers are generally prepared using a catalyst,comprising a transition metal compound and an organoaluminum compound,i.e., so-called Ziegler catalyst.

[0005] Propylene polymers prepared by the use of a titanium catalystcontaining a halogen-containing titanium catalyst component among theZiegler catalysts are excellent in moldability and rigidity, but theyhave such problems that they are poor in tensile elongation at break.Moreover, the titanium, catalyst causes a large amount of a catalystresidue in the resulting polymer because of low polymerizationactivities, and hence the molded article is sometimes colored ordeteriorated in sanitariness.

[0006] On the other hand, propylene polymers prepared by the use of ametallocene catalyst containing a transition metal compound catalystcomponent such as zirconocene are excellent in tensile elongation atbreak, but they have such problems that they are poor in moldability andrigidity (flexural modulus). As for the metallocene catalyst, however,the amount of the catalyst residue is small because of highpolymerization activities, and the molded article is never colored andis good in sanitariness.

[0007] Though the characteristics required for the propylene polymersvary depending on the molding methods or uses, generally required aremoldability, heat resistance, mechanical strength, high tensileelongation at break, impact resistance, etc. For satisfying theserequirements, researches on various compositions such as a compositionobtained by blending two or more kinds of propylene polymers and acomposition obtained by blending a propylene polymer and other syntheticresin have been made.

[0008] For example, blending of two kinds of propylene polymers whichare different in the molecular weight has been carried out in order toimprove physical properties of the propylene polymers prepared by theuse of a titanium catalyst. However, when two kinds of propylenepolymers produced by the use of a titanium catalyst are blended toprepare a propylene polymer composition, the tensile elongation at breakof the resulting composition is markedly lowered, though the moldabilitythereof is improved.

[0009] Further, adding of a soft polymer to a propylene polymer which isprepared by the use of a titanium catalyst has been carried out in orderto improve the tensile elongation at break and the impact resistance ofthe propylene polymer. The soft polymer used therefor is, for example,an ethylene/propylene random copolymer prepared by the use of a titaniumcatalyst or a vanadium catalyst. However, even if the propylene polymerprepared by the use of a titanium catalyst is blended with theethylene/propylene random copolymer prepared by the use of a titaniumcatalyst or the like, the resulting composition is not sufficientlyimproved in the tensile elongation at break and the impact resistance.

[0010] As described above, the conventional propylene polymercompositions are not always satisfactory in the properties such as heatresistance, mechanical strength and tensile elongation at break.

OBJECT OF THE INVENTION

[0011] The present invention has been accomplished in the light of theforegoing prior art technique, and an object of the present invention isto provide propylene polymer compositions which are excellent in heatresistance, mechanical strength, tensile elongation at break, etc. ascompared with the conventional propylene polymers or propylene polymercompositions.

SUMMARY OF THE INVENTION

[0012] The first propylene polymer composition of the inventioncomprises:

[0013] (A1) a propylene polymer, in an amount of 10 to 90% by weight,which is characterized in that:

[0014] (1) the propylene polymer is obtained by polymerizing propylenein the presence of an olefin polymerization catalyst comprising:

[0015] (i) (a) a compound of a Group IVB transition metal in theperiodic table containing a ligand having a cyclopentadienyl skeleton,and

[0016] (ii) at least one compound selected from the group consisting of

[0017] (b) an organoaluminum oxy-compound, and

[0018] (c) a compound which reacts with the transition metal compound(a) to form an ion pair,

[0019] (2) the propylene polymer has a melt flow rate (MFR), as measuredat 230° C. under a load of 2.16 kg, of 0.01 to 30 g/10 min, and

[0020] (3) the propylene polymer has a molecular weight distribution(Mw/Mn), as measured by gel permeation chromatography (GPC), of 2 to 3;and

[0021] (A2) a propylene polymer, in an amount of 10 to 90% by weight,which is characterized in that:

[0022] (1) the propylene polymer is obtained by polymerizing propylenein the presence of an olefin polymerization catalyst comprising:

[0023] (i) (a) a compound of a Group IVB transition metal in theperiodic table containing a ligand having a cyclopentadienyl skeleton,and

[0024] (ii) at least one compound selected from the group consisting of

[0025] (b) an organoaluminum oxy-compound, and

[0026] (c) a compound which reacts with the transition metal compound(a) to form an ion pair,

[0027] (2) the propylene polymer has a melt flow rate (MFR), as measuredat 230° C. under a load of 2.16 kg, of 30 to 0.1,000 g/10 min, and

[0028] (3) the propylene polymer has a molecular weight distribution(Mw/Mn), as measured by gel permeation chromatography (GPC), of 2 to 4;

[0029] a ratio ((A2)/(A1)) of the MFR of said propylene polymer (A2) tothe MFR of said propylene polymer (A1) being not less than 30.

[0030] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but alsomoldability.

[0031] The second propylene polymer composition of the inventioncomprises:

[0032] (A1) a propylene polymer, in an amount of 10 to 90 parts byweight, which is characterized in that:

[0033] (1) the propylene polymer is obtained by polymerizing propylenein the presence of an olefin polymerization catalyst comprising:

[0034] (i) (a) a compound of a Group IVB transition metal in theperiodic table containing a ligand having a cyclopentadienyl skeleton,and

[0035] (ii) at least one compound selected from the group consisting of

[0036] (b) an organoaluminum oxy-compound, and

[0037] (c) a compound which reacts with the transition metal compound(a) to form an ion pair,

[0038] (2) the propylene polymer has a melt flow rate (MFR), as measuredat 230. C under a load of. 2.16 kg, of 0.01 to 30 g/10 min, and

[0039] (3) the propylene polymer has a molecular weight distribution(Mw/Mn), as measured by gel permeation chromatography (GPC), of 2 to 3;

[0040] (A2) a propylene polymer, in an amount of 10 to 90 parts byweight, which is characterized in that:

[0041] (1) the propylene polymer is obtained by polymerizing propylenein the presence of an olefin polymerization catalyst comprising:

[0042] (i) (a) a compound of a Group IVB transition metal in theperiodic table containing a ligand having a cyclopentadienyl skeleton,and

[0043] (ii) at least one compound selected from the group consisting of

[0044] (b) an organoaluminum oxy-compound, and

[0045] (c) a compound which reacts with the transition metal compound(a) to form an ion pair,

[0046] (2) the propylene polymer has a melt flow rate (MFR), as measuredat 230° C. under a load of 2.16 kg, of 30 to 1,000 g/10 min, and

[0047] (3) the propylene polymer has a molecular weight distribution(Mw/Mn), as measured by gel permeation chromatography (GPC), of 2 to 4;and

[0048] (B) a soft polymer in an amount of 3 to 30 parts by weight;

[0049] a ratio ((A2)/(A1)) of the MFR of said propylene polymer (A2) tothe MFR of said propylene polymer (A1) being not less than 30.

[0050] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but alsomoldability and impact resistance.

[0051] The third propylene polymer composition of the inventioncomprises:

[0052] (A3) a propylene polymer, in an amount of 10 to 90% by weight,which is characterized in that:

[0053] (1) the propylene polymer is obtained by polymerizing propylenein the presence of an olefin polymerization catalyst comprising:

[0054] (d) a solid titanium catalyst component, and

[0055] (e) an organometallic compound catalyst component,

[0056] (2) the propylene polymer has a melt flow rate (MFR), as measuredat 230° C. under a load of 2.16 kg, of 0.01 to 30 g/10 min, and

[0057] (3) the propylene polymer has a molecular weight distribution(Mw/Mn), as measured by gel permeation chromatography (GPC), of 4 to 15;and

[0058] (A2) a propylene polymer, in an amount of 90 to 10% by weight,which is characterized in that:

[0059] (1) the propylene polymer is obtained by polymerizing propylenein the presence of an olefin polymerization catalyst comprising:

[0060] (i) (a) a compound of a Group IVB transition metal in theperiodic table containing a ligand having a cyclopentadienyl skeleton,and

[0061] (ii) at least one compound selected from the group consisting of

[0062] (b) an organoaluminum oxy-compound, and

[0063] (c) a compound which reacts with the transition metal compound(a) to form an ion pair,

[0064] (2) the propylene polymer has a melt flow rate (MFR), as measuredat 230° C. under a load of 2.16 kg, of 30 to 1,000 g/10 min, and

[0065] (3) the propylene polymer has a molecular weight distribution(Mw/Mn), as measured by gel permeation chromatography (GPC), of 2 to 4.

[0066] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but alsomoldability.

[0067] The fourth propylene polymer composition of the inventioncomprises:

[0068] (A3) a propylene polymer, in an amount of 10 to 90 parts byweight, which is characterized in that:

[0069] (1) the propylene polymer is obtained by polymerizing propylenein the presence of an olefin polymerization catalyst comprising:

[0070] (d) a solid titanium catalyst component, and

[0071] (e) an organometallic compound catalyst component,

[0072] (2) the propylene polymer has a melt flow rate (MFR), as measuredat 230° C. under a load of 2.16 kg, of 0.01 to 30 g/10 min, and

[0073] (3) the propylene polymer has a molecular weight distribution(Mw/Mn), as measured by gel permeation chromatography (GPC), of 4 to 15;

[0074] (A2) a propylene polymer, in an amount of 90 to 10 parts byweight, which is characterized in that:

[0075] (1) the propylene polymer is obtained by polymerizing propylenein the presence of an olefin polymerization catalyst comprising:

[0076] (i) (a) a compound of a Group IVB transition metal in theperiodic table containing a ligand having a cyclopentadienyl skeleton,and

[0077] (ii) at least one compound selected from the group consisting of

[0078] (b) an organoaluminum oxy-compound, and

[0079] (c) a compound which reacts with the transition metal compound(a) to form an ion pair,

[0080] (2) the propylene polymer has a melt flow rate (MFR), as measuredat 230° C. under a load of 2.16 kg, of 30 to 1,000 g/10 min, and

[0081] (3) the propylene polymer has a molecular weight distribution(Mw/Mn), as measured by gel permeation chromatography (GPC), of 2 to 4;and

[0082] (B) a soft polymer in an amount of 3 to 30 parts by weight.

[0083] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but alsomoldability and impact resistance.

[0084] The fifth propylene polymer composition of the inventioncomprises:

[0085] (A4) a propylene polymer, in an amount of 50 to 97% by weight,which is characterized in that:

[0086] (1) the propylene polymer is obtained by polymerizing propylenein the presence of an olefin polymerization catalyst comprising:

[0087] (d) a solid titanium catalyst component, and

[0088] (e) an organometallic compound catalyst component,

[0089] (2) the propylene polymer has a melt flow rate (MFR), as measuredat 230° C. under a load of 2.16 kg, of 0.01 to 50 g/10 min,

[0090] (3) the propylene polymer has a molecular weight distribution(Mw/Mn), as measured by gel permeation chromatography (GPC), of 4 to 15,and

[0091] (4) the propylene polymer has a crystallinity, as measured byX-ray diffractometry, of not less than 50%; and

[0092] (C) an ethylene/olefin random copolymer, in an amount of 3 to 50%by weight, which is characterized in that:

[0093] (1) the copolymer is obtained by copolymerizing ethylene and atleast one monomer selected from α-olefins of 3 to 20 carbon atoms andpolyenes of 5 to 20 carbon 1.5 atoms in the presence of an olefinpolymerization catalyst comprising:

[0094] (i) (f) a compound of a Group IVB transition metal in theperiodic table containing a ligand having a cyclopenta dienyl skeleton,

[0095] (ii) at least one compound selected from the group consisting of

[0096] (b) an organoaluminum oxy-compound, and

[0097] (g) a compound which reacts with the transition metal compound(f) to form an ion pair,

[0098] (2) the copolymer contains constituent units derived fromethylene in an amount of 20 to 80% by mol, and

[0099] (3) the copolymer has an intrinsic viscosity [η], as measured indecalin at 135° C., of 1.5 to 5 dl/g.

[0100] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but also impactresistance, particularly low-temperature impact resistance.

[0101] The sixth propylene polymer composition of the inventioncomprises:

[0102] (A5) a propylene homopolymer, in an amount of 5 to 95% by weight,which is obtained by polymerizing propylene in the presence of an olefinpolymerization catalyst comprising:

[0103] (i) (h) a transition metal compound represented by the followingformula (I), and

[0104] (ii) at least one compound selected from the group consisting of

[0105] (b) an organoaluminum oxy-compound, and

[0106] (i) a compound which reacts with the transition metal compound(h) to form an ion pair; and

[0107] (A6) a propylene polymer, in an amount of 5 to 95% by weight,which contains constituent units derived from propylene in an amount ofnot less than 90% by mol and is different from the propylene homopolymer(A5);

[0108] wherein M is a transition metal of Group IVa, Group Va or GroupVIa of the periodic table; R¹ is a hydrocarbon group of 2 to 6 carbonatoms; R² is an aryl group of 6 to 16 carbon atoms which may besubstituted with a halogen atom or a hydrocarbon group of 1 to 20 carbonatoms; X¹ and X² are each a hydrogen atom, a halogen atom, a hydrocarbongroup of 1 to 20 carbon atoms, a halogenated hydrocarbon group of 1 to20 carbon atoms, an oxygen-containing group or a sulfur-containinggroup; Y is a divalent hydrocarbon group of 1 to 20 carbon atoms, adivalent halogenated hydrocarbon group of 1 to 20 carbon atoms, adivalent silicon-containing group, a divalent germanium-containinggroup, a divalent tin-containing group, —O—, —CO—, —S—, SO—, —SO₂—,—NR³—, —P(R³)—, —P(O) (R³)—, —BR³—or —AlR³— (R³ is a hydrogen atom, ahalogen atom, a hydrocarbon group of 1 to 20 carbon atoms or ahalogenated hydrocarbon group of 1 to 20 carbon atoms).

[0109] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but alsomoldability.

[0110] The seventh propylene polymer composition of the inventioncomprises:

[0111] (A5) a propylene homopolymer, in an amount of 5 to 95% by weight,which is obtained by polymerizing propylene in the presence of an olefinpolymerization catalyst comprising:

[0112] (i) (h) a transition metal compound represented by the aboveformula (I), and

[0113] (ii) at least one compound selected from the group consisting of

[0114] (b) an organoaluminum oxy-compound, and

[0115] (i) a compound which reacts with the transition metal compound(h) to form an ion pair; and

[0116] (D) an olefin elastomer, in an amount of 5 to 95% by weight,which is characterized in that:

[0117] (1) the elastomer is a polymer or copolymer of at least onemonomer selected from olefins of 2 to 20 carbon atoms and polyenes of 5to 20 carbon atoms,

[0118] (2) the elastomer contains constituent units derived fromethylene, propylene, butene or 4-methyl-1-pentene in an amount of lessthan 90% by mol, and

[0119] (3) the elastomer has a glass transition temperature (Tg) of nothigher than 10° C.

[0120] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but also impactresistance.

[0121] The eighth propylene polymer composition of the inventioncomprises:

[0122] (A5) a propylene homopolymer, in an amount of 5 to 95% by weight,which is obtained by polymerizing propylene in the presence of an olefinpolymerization catalyst comprising:

[0123] (i) (h) a transition metal compound represented by the aboveformula (I), and

[0124] (ii) at least one compound selected from the group consisting of

[0125] (b) an organoaluminum oxy-compound, and

[0126] (i) a compound which reacts with the transition metal compound(h) to form an ion pair; and

[0127] (E) an olefin polymer, in an amount of 5 to 95% by weight, whichcontains constituent units derived from one monomer selected from thegroup consisting of ethylene, butene and 4-methyl-1-pentene in an amountof not less than 90% by mol.

[0128] Such propylene polymer composition is excellent in heatresistance, rigidity and tensile elongation at break.

[0129] The ninth propylene polymer composition of the inventioncomprises:

[0130] (A5) a propylene homopolymer which is obtained by polymerizingpropylene in the presence of an olefin polymerization catalystcomprising:

[0131] (i) (h) a transition metal compound represented by the aboveformula (I), and

[0132] (ii) at least one compound selected from the group consisting of

[0133] (b) an organoaluminum oxy-compound, and

[0134] (i) a compound which reacts with the transition metal compound(h) to form an ion pair;

[0135] (A6) a propylene polymer which contains constituent units derivedfrom propylene in an amount of not less than 90% by mol and is differentfrom the propylene homopolymer (A5); and

[0136] (D) an olefin elastomer which is characterized in that:

[0137] (1) the elastomer is a polymer or copolymer of at least onemonomer selected from olefins of 2 to 20 carbon atoms and polyenes of 5to 20 carbon atoms,

[0138] (2) the elastomer contains constituent units derived fromethylene, propylene, butene or 4-methyl-1-pentene in an amount of lessthan 90% by mol, and

[0139] (3) the elastomer has a glass transition temperature (Tg) of nothigher than 10° C.;

[0140] said propylene polymer composition containing the propylenehomopolymer (A5) in an amount of 5 to 95% by weight, the propylenepolymer (A6) in an amount of not more than 95% by weight and the olefinelastomer (D) in an amount of not more than 95% by weight.

[0141] Such propylene polymer composition is excellent in not onlyheat-resistance, rigidity and tensile elongation at break but alsomoldability and impact resistance.

[0142] The tenth propylene polymer composition of the inventioncomprises:

[0143] (A5) a propylene homopolymer which is obtained by polymerizingpropylene in the presence of an olefin polymerization catalystcomprising:

[0144] (i) (h) a transition metal compound represented by the aboveformula (I), and

[0145] (ii) at least one compound selected from the group consisting of

[0146] (b) an organoaluminum oxy-compound, and

[0147] (i) a compound which reacts with the transition metal compound(h) to form an ion pair;

[0148] (A6) a propylene polymer which contains constituent units derivedfrom propylene in an amount of not less than 90% by mol and is differentfrom the propylene homopolymer (A5); and

[0149] (E) an olefin polymer which contains constituent units derivedfrom one monomer selected from the group consisting of ethylene, buteneand 4-methyl-1-pentene in an amount of not less than 90% by mol;

[0150] said propylene polymer composition containing the propylenehomopolymer (A5) in an amount of 5 to 95% by weight, the propylenepolymer (A6) in an amount of not more than 95% by weight and the olefinpolymer (E) in an amount of not more than 95% by weight.

[0151] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but alsomoldability.

[0152] The eleventh propylene polymer composition of the inventioncomprises:

[0153] (A5) a propylene homopolymer which is obtained by polymerizingpropylene in the presence of an olefin polymerization catalystcomprising:

[0154] (i) (h) a transition metal compound represented by the aboveformula (I), and

[0155] (ii) at least one compound selected from the group consisting of

[0156] (b) an organoaluminum oxy-compound, and

[0157] (i) a compound which reacts with the transition metal compound(h) to form an ion pair;

[0158] (D) an olefin elastomer which is characterized in that:

[0159] (1) the elastomer is a polymer or copolymer of at least onemonomer selected from olefins of 2 to 20 carbon atoms and polyenes of 5to 20 carbon atoms,

[0160] (2) the elastomer contains constituent units derived fromethylene, propylene, butene or 4-methyl-1-pentene in an amount of lessthan 90% by mol, and

[0161] (3) the elastomer has a glass transition temperature (Tg) of nothigher than 10° C.; and

[0162] (E) an olefin polymer which contains constituent units derivedfrom one monomer selected from the group consisting of ethylene, buteneand 4-methyl-1-pentene in an amount of not less than 90% by mol;

[0163] said propylene polymer composition containing the propylenehomopolymer (A5) in an amount of 5 to 95% by weight, the olefinelastomer (D) in an amount of not more than 95% by weight and the olefinpolymer (E) in an amount of not more than 95% by weight.

[0164] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but also impactresistance.

[0165] The twelfth propylene polymer composition of the inventioncomprises:

[0166] (A5) a propylene homopolymer which is obtained by polymerizingpropylene in the presence of an olefin polymerization catalystcomprising:

[0167] (i) (h) a transition metal compound represented by the aboveformula (I), and

[0168] (ii) at least one compound selected from the group consisting of

[0169] (b) an organoaluminum oxy-compound, and

[0170] (i) a compound which reacts with the transition metal compound(h) to form an ion pair;

[0171] (A6) a propylene polymer which contains constituent units derivedfrom propylene in an amount of not less than 90% by mol and is differentfrom the propylene homopolymer (A5);

[0172] (D) an olefin elastomer which is characterized in that:

[0173] (1) the elastomer is a polymer or copolymer of at least onemonomer selected from olefins of 2 to 20 carbon atoms and polyenes of 5to 20 carbon atoms,

[0174] (2) the elastomer contains constituent units derived fromethylene, propylene, butene or 4-methyl-1-pentene in an amount of lessthan 90% by mol, and

[0175] (3) the elastomer has a glass transition temperature (Tg) of nothigher than 10° C.; and

[0176] (E) an olefin polymer which contains constituent units derivedfrom one monomer selected from the group consisting of ethylene, buteneand 4-methyl-1-pentene in an amount of not less than 90% by mol;

[0177] said propylene polymer composition containing the propylenehomopolymer (A5) in an amount of 5 to 95% by weight, the propylenepolymer (A6) in an amount of not more than 95% by weight, the olefinelastomer (D) in an amount of not more than 95% by weight and the olefinpolymer (E) in an amount of not more than 95% by weight.

[0178] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but alsomoldability and impact resistance.

[0179] The thirteenth propylene polymer composition of the inventioncomprises:

[0180] (A7) a propylene copolymer, in an amount of 5 to 95% by weight,which is characterized in that:

[0181] (1) the propylene copolymer is obtained by copolymerizingpropylene and at least one α-olefin selected from ethylene and α-olefinsof 4 to 20 carbon atoms in the presence of an olefin polymerizationcatalyst comprising:

[0182] (i) (h) a transition metal compound represented by the aboveformula (I), and

[0183] (ii) at least one compound selected from the group consisting of

[0184] (b) an organoaluminum oxy-compound, and

[0185] (i) a compound which reacts with the transition metal compound(h) to form an ion pair, and

[0186] (2) the propylene copolymer contains constituent units derivedfrom propylene in an amount of not less than 90% by mol; and

[0187] (A6) a propylene polymer, in an amount of 5 to 95% by weight,which contains constituent units derived from propylene in an amount ofnot less than 90% by mol and is different from the propylene copolymer(A7).

[0188] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but alsomoldability.

[0189] The fourteenth propylene polymer composition of the inventioncomprises:

[0190] (A7) a propylene copolymer, in an amount of 5 to 95% by weight,which is characterized in that:

[0191] (1) the propylene copolymer is obtained by copolymerizingpropylene and at least one α-olefin selected from ethylene and α-olefinsof 4 to-20 carbon atoms in the presence of an olefin polymerizationcatalyst comprising:

[0192] (i) (h) a transition metal compound represented by the aboveformula (I), and

[0193] (ii) at least one compound selected from the group consisting of

[0194] (b) an organoaluminum oxy-compound, and

[0195] (i) a compound which reacts with the transition metal compound(h) to form an ion pair, and

[0196] (2) the propylene copolymer contains constituent units derivedfrom propylene in an amount of not less than 90% by mol; and

[0197] (D) an olefin elastomer, in an amount of 5 to 95% by weight,which is characterized in that:

[0198] (1) the elastomer is a polymer or copolymer of at least onemonomer selected from olefins of 2 to 20 carbon atoms and polyenes of 5to 20 carbon atoms,

[0199] (2) the elastomer contains constituent units derived fromethylene, propylene, butene or 4-methyl-1-pentene in an amount of lessthan 90% by mol, and

[0200] (3) the elastomer has a glass transition temperature (Tg) of nothigher than 10° C.

[0201] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but also impactresistance.

[0202] The fifteenth propylene polymer composition of the inventioncomprises:

[0203] (A7) a propylene copolymer, in an amount of 5 to 95% by weight,which is characterized in that:

[0204] (1) the propylene copolymer is obtained by copolymerizingpropylene and at least one α-olefin selected from ethylene and α-olefinsof 4 to 20 carbon atoms in the presence of an olefin polymerizationcatalyst comprising:

[0205] (i) (h) a transition metal compound represented by the aboveformula (I), and

[0206] (ii) at least one compound selected from the group consisting of

[0207] (b) an organoaluminum oxy-compound, and

[0208] (i) a compound which reacts with the transition metal compound(h) to form an ion pair, and

[0209] (2) the propylene copolymer contains constituent units derivedfrom propylene in an amount of not less than 90% by mol; and

[0210] (E) an olefin polymer, in an amount of 5 to 95% by weight, whichcontains constituent units derived from one monomer selected from thegroup consisting of ethylene, butene and 4-methyl-1-pentene in an amountof not less than 90% by mol.

[0211] Such propylene polymer composition is excellent in heatresistance, rigidity and tensile elongation at break.

[0212] The sixteenth propylene polymer composition of the inventioncomprises:

[0213] (A7) a propylene copolymer which is characterized in that:

[0214] (1) the propylene copolymer is obtained by copolymerizingpropylene and at least one α-olefin selected from ethylene and α-olefinsof 4 to 20 carbon atoms in the presence of an olefin polymerizationcatalyst comprising:

[0215] (i) (h) a transition metal compound represented by the aboveformula (I), and

[0216] (ii) at least one compound selected from the group consisting of

[0217] (b) an organoaluminum oxy-compound, and

[0218] (i) a compound which reacts with the transition metal compound(h) to form an ion pair, and

[0219] (2) the propylene copolymer contains constituent units derivedfrom propylene in an amount of not less than 90% by mol;

[0220] (A6) a propylene polymer which contains constituent units derivedfrom propylene in an amount of not less than 90% by mol and is differentfrom the propylene copolymer (A7); and

[0221] (D) an olefin elastomer which is characterized in that:

[0222] (1) the elastomer is a polymer or copolymer of at least onemonomer selected from olefins of 2 to 20 carbon atoms and polyenes of 5to 20 carbon atoms,

[0223] (2) the elastomer contains constituent-units derived fromethylene, propylene, butene or 4-methyl-1-pentene in an amount of lessthan 90% by mol, and

[0224] (3) the elastomer has a glass transition temperature (Tg) of nothigher than 10° C.;

[0225] said propylene polymer composition containing the propylenecopolymer (A7) in an amount of 5 to 95% by weight, the propylene polymer(A6) in an amount of not more than 95% by weight and the olefinelastomer (D) in an amount of not more than 95% by weight.

[0226] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but alsomoldability and impact resistance.

[0227] The seventeenth propylene polymer composition of the inventioncomprises:

[0228] (A7) a propylene copolymer which is characterized in that:

[0229] (1) the propylene copolymer is obtained by copolymerizingpropylene and at least one α-olefin selected from ethylene and α-olefinsof 4 to 20 carbon atoms in the presence of an olefin polymerizationcatalyst comprising:

[0230] (i) (h) a transition metal compound represented by the aboveformula (I), and

[0231] (ii) at least one compound selected from the group consisting of

[0232] (b) an organoaluminum oxy-compound, and

[0233] (i) a compound which reacts with the transition metal compound(h) to form an ion pair, and

[0234] (2) the propylene copolymer contains constituent units derivedfrom propylene in an amount of not less than 90% by mol;

[0235] (A6) a propylene polymer which contains constituent units derivedfrom propylene in an amount of not less than 90. % by mol and isdifferent from the propylene copolymer (A7); and

[0236] (E) an olefin polymer which contains constituent units derivedfrom one monomer selected from the group consisting of ethylene, buteneand 4-methyl-1-pentene in an amount of not less than 90% by mol;

[0237] said propylene polymer composition containing the propylenecopolymer (A7) in an amount of 5 to 95% by weight, the propylene polymer(A6) in an amount of not more than 95% by weight and the olefin polymer(E) in an amount of not more than 95% by weight.

[0238] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but alsomoldability.

[0239] The eighteenth propylene polymer composition of the inventioncomprises:

[0240] (A7) a propylene copolymer which is characterized in that:

[0241] (1) the propylene copolymer is obtained by copolymerizingpropylene and at least one α-olefin selected from ethylene and α-olefinsof 4 to 20 carbon atoms in the presence of olefins polymerizationcatalyst comprising:

[0242] (i) (h) a transition metal compound represented by the aboveformula (I), and

[0243] (ii) at least one compound selected from the, group consisting of

[0244] (b) an organoaluminum oxy-compound, and

[0245] (i) a compound which reacts with the transition metal compound(h) to form an ion pair, and

[0246] (2) the propylene copolymer contains constituent units derivedfrom propylene in an amount of not less than 90% by mol;

[0247] (D) an olefin elastomer which is characterized in that:

[0248] (1) the elastomer is a polymer or copolymer of at least onemonomer selected from olefins of 2 to 20 carbon atoms and polyenes of 5to 20 carbon atoms,

[0249] (2) the elastomer contains constituent units derived fromethylene, propylene, butene or 4-methyl-1-pentene in an amount of lessthan 90% by mol, and

[0250] (3) the elastomer has a glass transition temperature (Tg) of nothigher than 10° C.; and

[0251] (E) an olefin polymer which contains constituent units derivedfrom one monomer selected from the group consisting of ethylene, buteneand 4-methyl-1-pentene in an amount of not less than 90% by mol;

[0252] said propylene polymer composition containing the propylenecopolymer (A7) in an amount of 5 to 95% by weight, the olefin elastomer(D) in an amount of not more than 95% by weight and the olefin polymer(E) in an amount of not more than 95% by weight.

[0253] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but also impactresistance.

[0254] The nineteenth propylene polymer composition of the inventioncomprises:

[0255] (A7) a propylene copolymer which is characterized in that:

[0256] (1) the propylene copolymer is obtained by copolymerizingpropylene and at least one α-olefin selected from ethylene and α-olefinsof 4 to 20 carbon atoms in the presence of an olefin polymerizationcatalyst comprising:

[0257] (i) (h) a transition metal compound represented by the aboveformula (I), and

[0258] (ii) at least one compound selected from the group consisting of

[0259] (b) an organoaluminum oxy-compound, and

[0260] (i) a compound which reacts with the transition metal compound(h) to form an ion pair, and

[0261] (2) the propylene copolymer contains constituent units derivedfrom propylene in an amount of not less than 90% by mol;

[0262] (A6) a propylene polymer which contains constituent units derivedfrom propylene in an amount of not less than 90% by mol and is differentfrom the propylene copolymer (A7);

[0263] (D) an olefin elastomer which is characterized in that:

[0264] (1) the elastomer is a polymer or copolymer of at least onemonomer selected from olefins of 2 to 20 carbon atoms and polyenes of 5to 20 carbon atoms,

[0265] (2) the elastomer contains constituent units derived fromethylene, propylene, butene or 4-methyl-1-pentene in an amount of lessthan 90% by mol, and

[0266] (3) the elastomer has a glass transition temperature (Tg) of nothigher than 10° C.; and

[0267] (E) an olefin polymer which contains constituent units derivedfrom one monomer selected from the group consisting of ethylene, buteneand 4-methyl-1-pentene in an amount of not less than 90% by mol;

[0268] said propylene polymer composition containing the propylenecopolymer (A7) in an amount of 5 to 95% by weight, the propylene polymer(A6) in an amount of not more than 95% by weight, the olefin elastomer(D) in an amount of not more than 95% by weight and the olefin polymer(E) in an amount of not more than 95% by weight.

[0269] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but alsomoldability and impact resistance.

BRIEF DESCRIPTION OF THE DRAWINGS

[0270]FIG. 1 is a view illustrating steps of a process for preparing anolefin polymerization catalyst which is used for the preparation of thepropylene polymer (A1) and the propylene polymer (A2).

[0271]FIG. 2 is a view illustrating steps of a process for preparing anolefin polymerization catalyst which is used for the preparation of thepropylene polymer (A3) and the propylene polymer (A4).

[0272]FIG. 3 is a view illustrating steps of a process for preparing anolefin polymerization catalyst which is used for the preparation of theethylene/olefin random copolymer (C).

[0273]FIG. 4 is a view illustrating steps of a process for preparing anolefin polymerization catalyst which is used for the preparation of thepropylene homopolymer (A5) and the propylene copolymer (A7).

DETAILED DESCRIPTION OF THE INVENTION

[0274] The propylene polymer compositions according to the presentinvention will be described in detail hereinafter.

The first Propylene Polymer Composition

[0275] The first propylene polymer composition comprises:

[0276] (A1) a propylene polymer which is characterized in that:

[0277] the propylene polymer is obtained by polymerizing propylene inthe presence of an olefin polymerization catalyst comprising:

[0278] (i) (a) a compound of a Group IVB transition metal in theperiodic table containing a ligand having a cyclopentadienyl skeleton,and

[0279] (ii) at least one compound selected from the group consisting of

[0280] (b) an organoaluminum oxy-compound, and

[0281] (c) a compound which reacts with the transition metal compound(a) to form an ion pair, the propylene polymer has a melt flow rate(MFR), as measured at 230° C. under a load of 2.16 kg, of 0.01 to 30g/10 min, and

[0282] the propylene polymer has a molecular weight distribution(Mw/Mn), as measured by gel permeation chromatography (GPC), of 2 to 3;and

[0283] (A2) a propylene polymer which is characterized in that:

[0284] the propylene polymer is obtained by polymerizing propylene inthe presence of an olefin polymerization catalyst comprising:

[0285] (i) (a) a compound of a Group IVB transition metal in theperiodic table containing a ligand having a cyclopentadienyl skeleton,and

[0286] (ii) at least one compound selected from the group consisting of

[0287] (b) an organoaluminum oxy-compound, and

[0288] (c) a compound which reacts with the transition metal compound(a) to form an ion pair,

[0289] the propylene polymer has a melt flow rate (MFR), as measured at230° C. under a load of 2.16 kg, of 30 to 1,000 g/10 min, and

[0290] the propylene polymer has a molecular weight distribution(Mw/Mn), as measured by GPC, of 2 to 4.

[0291] In this propylene polymer composition, the ratio ((A2)/(A1)) ofthe MFR of said propylene polymer (A2) to the MFR of said propylenepolymer (A1) is not less than 30.

[0292] Propylene Polymer (A1)

[0293] The propylene polymer (A1) for constituting the first propylenepolymer composition is a propylene homopolymer or a propylene copolymerobtained by the use of an olefin polymerization catalyst comprising atransition metal compound (a) and at least one compound selected fromthe group consisting of an organoaluminum oxy-compound (b) and acompound (C), all compounds being described later.

[0294] The propylene polymer (A1) is desired to have MFR, as measured at230° C. under a load of 2.16 kg, of 0.01 to 30 g/10 min, preferably 0.5to 5.0 g/10 min, and Mw/Mn; as measured by GPC, of 2 to 3.

[0295] Further, the propylene polymer (A1) is desired to have anintrinsic viscosity [TI] of 1.3 to 5.0 dl/g, preferably 2.0 to 4.0 dl/g,a weight-average molecular weight of 12×10⁴ to 100×10⁴, preferably20×10⁴ to 70×10⁴, and a crystallinity, as measured by X-raydiffractometry, of not less than 40%, preferably not less than 50%.

[0296] The propylene polymer (A1) may contain constituent units derivedfrom other monomers than propylene, such as ethylene and α-olefins of 4to 20 carbon atoms, e.g., 1-butene, 1-pentene, 1-hexene,4-methyl-1-pentene, 1-octene, 1-decene, 1-dodecene, 1-tetradecene,1-hexadecene, 1-octadecene and 1-eicosene, in an amount of not more than10% by mol.

[0297] Propylene Polymer (A2)

[0298] The propylene polymer (A2) for constituting the first propylenepolymer composition is a propylene homopolymer or a propylene copolymerobtained by the use of an olefin polymerization catalyst comprising atransition metal-compound (a) and at least one compound selected fromthe group consisting of an organoaluminum oxy-compound (b) and acompound (C), all compounds being described later.

[0299] The propylene polymer (A2) is desired to have MFR, as measured at230° C. under a load of 2.16 kg, of 30 to 1,000 g/10 min, preferably 50to 200 g/10 min, and Mw/Mn, as measured by GPC, of 2 to 4.

[0300] Further, the propylene polymer (A2) is desired to have anintrinsic viscosity [η] of not less than 0.5 and less than 1.3 dl/g,preferably not less than 0.8 and less than 1.3 dl/g, a weight-averagemolecular weight of 5×10³ to 15×10⁴, preferably 1×10⁴ to 12×10⁴, and acrystallinity, as measured by X-ray diffractometry, of not less than40%, preferably not less than-50%.

[0301] The propylene polymer (A2) may contain constituent units derivedfrom other monomers than propylene, which are exemplified for thepropylene polymer (A1), in an amount of not more than 5% by mol.

[0302] Propylene Polymer Composition

[0303] The first propylene polymer composition comprises the propylenepolymer (A1) and the propylene polymer (A2). In this composition, it isdesired that the propylene polymer (A1) is contained in an amount of 10to 90% by weight, preferably 30 to 70% by weight; and the propylenepolymer (A2) is contained in an amount of 10 to 90% by weight,preferably 30 to 70% by weight. A ratio [(A2)/(A1)] of the MFR of thepropylene polymer (A2) to the MFR of the propylene polymer (A1) is notless than 30, preferably in the range of 40 to 300, more preferably 50to 100.

[0304] The first propylene polymer composition is desired to have MFR,as measured at 230° C. under a load of 2.16 kg, of 1 to 100 g/10 min,preferably 5 to 50 g/10 min. In this composition, Mw/Mn of all thepropylene components for constituting the composition is desirably inthe range of 4 to 15.

[0305] The density of the first propylene polymer composition is desiredto be in the range of 0.89 to 0.92 g/cm³, preferably 0.90 to 0.92g/cm^(3.)

[0306] The heat distortion temperature (HDT) thereof is desired to benot lower than 95° C., preferably in the range of 100 to 140° C.

[0307] The flexural modulus (FM) thereof is desired to be in the rangeof 12,000 to 19,000 kg/cm², preferably 14,000 to 18,000 kg/cm².

[0308] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 2 to 4 kg·cm/cm, preferably 2 to 3 kg·cm/cm.

[0309] The tensile elongation at break (EL) thereof is desired to be inthe range of 100 to 500%, preferably 200 to 400%.

[0310] The first propylene polymer composition may contain additives, ifnecessary, such as weathering stabilizer, heat stabilizer, antistaticagent, anti-slip agent, anti-blocking agent, anti-fogging agent,lubricant, pigment, dye, nucleating agent, plasticizer, anti-agingagent, hydrochloric acid absorber and antioxidant, with the proviso thatthe object of the invention is not marred.

[0311] The first propylene polymer composition can be prepared byconventionally known processes, for example, by the following ones.

[0312] (1) A process comprising mechanically blending the propylenepolymer (A1), the propylene polymer (A2) and, if desired, othercomponents by means of an extruder, a kneader, etc.

[0313] (2) A process comprising dissolving the propylene polymer (A1),the propylene polymer (A2)- and, if desired, other components in anappropriate good solvent (e.g., hydrocarbon solvents such as hexane,heptane, decane, cyclohexane, benzene, toluene and xylene), and removingthe solvent.

[0314] (3) A process comprising individually dissolving the propylenepolymer (A1), the propylene polymer (A2) and, if desired, othercomponents in appropriate good solvents respectively to give solutions,then mixing the solutions, and removing the solvent.

[0315] (4) A process comprising conducting the above processes (1) to(3) in combination.

[0316] (5) A process comprising conducting the polymerization in two ormore steps having different reaction conditions, in the first step ofwhich the propylene polymer (A1) is prepared, and in another step ofwhich the propylene polymer (A2) is prepared; alternatively, comprisingusing plural polymerizers, in one polymerizer of which the propylenepolymer (A1) is prepared, and in another polymerizer of which thepropylene polymer (A2) is prepared.

[0317] The first propylene polymer composition as mentioned above isexcellent in not only heat resistance, rigidity and tensile elongationat break but also moldability. Further, since the amount of the catalystresidue in the polymer composition is small, the article molded from thecomposition is never colored and is good in sanitariness.

[0318] Next, the olefin polymerization catalyst used in the preparationof the propylene polymer (A1) and the, propylene polymer (A2) and theprocess for preparing the propylene polymer (A1) and the propylenepolymer (A2) are described.

[0319] The propylene polymer (A1) and the propylene polymer (A2) can beprepared by polymerizing propylene in the presence of an olefinpolymerization catalyst [olefin polymerization catalyst (l)] comprising:

[0320] (i) (a) a compound of a Group IVB transition metal in theperiodic table containing a ligand having a, cyclopentadienyl skeleton,and

[0321] (ii) at least one compound selected from the group consisting of

[0322] (b) an organoaluminum oxy-compound, and

[0323] (c) a compound which reacts with the transition metal compound(a) to form an ion pair.

[0324]FIG. 1 illustrates steps of a process for preparing the olefinpolymerization catalyst which is used for the preparation of thepropylene polymer (A1) and the propylene polymer (A2).

[0325] Examples of the compound (a) of the Group IVB transition metal ofthe periodic table which contains a ligand having a cyclopentadienylskeleton include the transition metal compound represented by thefollowing formula (Ia) and the transition metal compound represented bythe following formula (I).

ML_(x)  (Ia)

[0326] wherein M is a transition metal atom selected from the groupconsisting of titanium, zirconium, hafnium, vanadium, niobium, tantalumand chromium, preferably titanium, zirconium or hafnium, and x is avalence of the transition metal atom.

[0327] L is a ligand coordinating to the transition metal, at least oneof L is a ligand having a cyclopentadienyl skeleton, and preferably atleast two of L are ligands having a cyclopentadienyl skeleton.

[0328] The ligands having a cyclopentadienyl skeleton are, for example,cyclopentadienyl group, indenyl group, 4,5,6,7-tetrahydroindenyl group,4,5,6,6a-tetrahydropentarenyl group, 7,8-dihydro-3H.6H-as-indacenylgroup and fluorenyl group. These groups as exemplified above may besubstituted with an alkyl group, an aryl group, an aralkyl group, atrialkylsilyl group, a halogen atom, an alkoxy group, an aryloxy group,a linear alkylene group or a cyclic alkylene group. Further, thesegroups having a cyclopentadienyl skeleton may form ring condensate withbenzene ring, naphthalene ring, acenaphthene ring or indene ring.

[0329] Of the ligands coordinating with the transition metal atom,preferred is a ligand having an indenyl skeleton, and particularlypreferred is ligand having a substituted indenyl skeleton.

[0330] When the transition metal compound represented by the abovegeneral formula (Ia) contains 2 or more ligands each having acyclopentadienyl skeleton, the two ligands out of them may be linkedtogether through an alkylene group such as ethylene or propylene;

[0331] a substituted alkylene group such as 1,2-di(methyl)ethylene;

[0332] a cycloalkylene group such as 1,4-cyclohexylene or1,3-cyclopentylene;

[0333] a substituted alkylidene group such as isopropylidene ordiphenylmethylene;

[0334] a silylene group;

[0335] a substituted silylene group such as dimethylsilylene,diphenylsilylene or methylphenylsilylene;

[0336] a germyl group;

[0337] —P(Ra)—, —P(O) (R^(b))—, SO₂N—(R^(c))— or Sn(R^(d) ₂)— [whereineach of R^(a), R^(c) and R^(d) ₂ is an alkyl group, and R^(b) is an arylgroup].

[0338] Of these, particularly preferred is ligand linked togetherthrough a substituted silylene group such as dimethylsilylene group,diphenylsilylene group or methylphenylsilylene group.

[0339] Example the ligands L other than those having a cyclopentadienylskeleton may include

[0340] a hydrocarbon group of 1-10 carbon atoms such as an alkyl group(e.g. methyl group, ethyl group, propyl group, isopropyl group, butylgroup, propyl group, pentyl group or neopentyl group), a cycloalkylgroup (e.g. cyclopentyl group or cyclohexyl group), an aryl group (e.g.phenyl group, tolyl group or mesityl group) and an aralkyl group (e.g.benzyl or neophyl),

[0341] an alkoxy group of 1-10 carbon atoms such as methoxy group,ethoxy group, propoxy group or butoxy group,

[0342] an aryloxy group of 6-10 carbon atoms such as phenoxy group,

[0343] a ligand represented by —OSO₂Re or —CH₂SiRe₃ (wherein R^(e) is ahydrocarbon group of 1-10 carbon atoms) such as mesitylsulfonate,phenylsulfonate, benzylsulfonate, methylsulfonate, p-toluenesulfonate ortrifluoromethanesulfonate,

[0344] a halogen atom such as fluorine, chlorine, bromine or iodine, and

[0345] hydrogen atom.

[0346] When the transition metal compound contains 2 or more ligandsother than those having a cyclopentadienyl skeleton, each ligand may bethe same or different.

[0347] When the valence of the transition metal atom is, for example, 4,the transition metal compound represented by the above formula (Ia) isrepresented by the following formula (Ib) in more detail.

R⁴ _(k)R⁵ _(l)R⁶ _(m)R⁷ _(n)M  (Ib)

[0348] wherein M represents the above mentioned transition metal atom,R⁴ represents a ligand having a cyclopentadienyl skeleton as in theabove formula (Ia), R⁵, R⁶ and R⁷ each represent a ligand having acyclopentadienyl skeleton or a ligand L other than those having acyclopentadienyl skeleton, k is an integer of 1 or more, and k+l+m+n=4.

[0349] In the present invention, there is used preferably a transitionmetal compound having the above-mentioned formula (Ib) in which at leasttwo of R⁴, R⁵, R⁶ and R⁷ are the substituted indenyl groups. In thiscase, these groups are prefereably linked together through a group as inthe above formula (Ia).

[0350] Exemplified below are the transit-ion metal compounds wherein Mis zirconium.

[0351] rac-ethylene-bis{1-(2-methylindenyl)}zirconium dichloride,

[0352] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiumdichloride,

[0353] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconium dihydride,

[0354] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiumdifluoride,

[0355] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconium dibromide,

[0356] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconium diiodide,

[0357] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiumdimethoxide,

[0358] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiumdi-n-butoxide,

[0359] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiumdiphenoxide,

[0360] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiumdi-t-butoxide,

[0361] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconium dimethyl,

[0362] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiumdineopentyl,

[0363] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiumditrimethylsilylmethyl,

[0364] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiumditosylate,

[0365] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiumdimesilate,

[0366] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiumdi(mesitylsulfonate),

[0367] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiumdi(phenylsulfonate),

[0368] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiumdi(benzylsulfonate),

[0369] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiumdi(trifluoromethanesulfonate),

[0370] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiummonochloride monohydride,

[0371] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiummonochloride monofluoride,

[0372] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiummonochloride monobromide,

[0373] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiummonochloride monoiodide,

[0374] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiummonochloride monomethoxide,

[0375] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiummonochloride mono-n-butoxide,

[0376] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiummonochloride monophenoxide,

[0377] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiummonochloride mono-t-butoxide,

[0378] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiummonochloride monomethyl,

[0379] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiummonochloride mononeopentyl,

[0380] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiummonochloride monotrimethylsilylmethyl,

[0381] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiummonochloride monotosylate,

[0382] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiummonochloride monomesilate,

[0383] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiummonochloride mono(mesitylsulfonate),

[0384] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiummonochloride mono(phenylsulfonate),

[0385] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiummonochloride mono(benzylsulfonate),

[0386] rac-dimethylsilylene-bis{1-(2-methylindenyl)}zirconiummonochloride mono(trifluoromethanesulfonate),

[0387] rac-diphenylsilylene-bis{1-(2-methylindenyl)}zirconiumdichloride,

[0388] rac-methylphenylsilylene-bis{1-(2-methylindenyl)}zirconiumdichloride,

[0389] rac-silylene-bis{1-(2-methylindenyl)}zirconium dichloride,

[0390] rac-dimethylgermylene-bis{1-(2-methylindenyl)}zirconiumdichloride,

[0391] rac-phenylphosphinylene-bis{1-(2-methylindenyl)}zirconiumdichloride,

[0392] rac-ethylene-bis{1-(2,4-dimethylindenyl)}zirconium dichloride,

[0393] rac-ethylene-bis{1-(2-methyl, 4-isopropylindenyl)}zirconiumdichloride,

[0394] rac-dimethylsilylene-bis{1-(2,4-dimethylindenyl)}zirconiumdichloride,

[0395] rac-dimethylsilylene-bis{1-(2-methyl, 4-ethylindenyl)}zirconiumdichloride,

[0396] rac-dimethylsilylene-bis{1-(2-methyl,4-n-propylindenyl)}zirconium dichloride,

[0397] rac-dimethylsilylene-bis{1-(2-methyl, isopropylindenyl)}zirconiumdichloride,

[0398] rac-dimethylsilylene-bis{1-(2-methyl-4-n-butylindenyl)}zirconiumdichloride,

[0399] rac-dimethylsilylene-bis{1-(2-methyl, 4-1-butylindenyl)}zirconiumdichloride,

[0400] rac-dimethylsilylene-bis{1-(2-methyl, 4-t-butylindenyl)}zirconiumdichloride,

[0401] rac-dimethylsilylene-bis{1-(2-methyl,4-trimethylsilylindenyl)}zirconium dichloride,

[0402] rac-dimethylsilylene-bis{1-(2-ethyl-4-isopropylindenyl)}zirconiumdichloride,

[0403] rac-dimethylsilylene-bis{1-(2-n-propyl,4-isopropylindenyl)}zirconium dichloride,

[0404] rac-dimethylsilylene-bis{1-(2-1-propyl,4-isopropylindenyl)}zirconium dichloride,

[0405] rac-dimethylsilylene-bis{1-(2-n-butyl,4-isopropylindenyl)}zirconium dichloride,

[0406] rac-dimethylsilylene-bis{1-(2-1-butyl,4-isopropylindenyl)}zirconium dichloride,

[0407] rac-dimethylsilylene-bis{1-(2-t-butyl,4-isopropylindenyl)}zirconium dichloride,

[0408] rac-dimethylsilylene-bis{1-(2-trimethylsilyl,4—isopropylindenyl)}zirconium dichloride,

[0409] rac-dimethylsilylene-bis{1-(2-phenyl,4-isopropylindenyl)}zirconium dichloride,

[0410] rac-diphenylsilylene-bis{1-(2,4-dimethylindenyl)}zirconiumdichloride,

[0411] rac-diphenylsilylene-bis{1-(2-methyl,4-isopropylindenyl)}zirconium dichloride,

[0412] rac-methylphenylsilylene-bis{1-(2,4-dimethylindenyl)}zirconiumdichloride,

[0413] rac-methylphenylsilylene-bis{1-(2-methyl,4-isopropylindenyl)}zirconium dichloride,

[0414] rac-ethylene-bis{1-(2,5-dimethylindenyl)}zirconium dichloride,

[0415] rac-ethylene-bis{1-(2-methyl, 5-isopropylindenyl)}zirconiumdichloride,

[0416] rac-dimethylsilylene-bis{1-(2,5-dimethylindenyl)}zirconiumdichloride,

[0417] rac-dimethylsilylene-bis{1-(2-methyl,5-isopropylindenyl)}zirconium dichloride,

[0418] rac-diphenylsilylene-bis{1-(2,5-dimethylindenyl)}zirconiumdichloride,

[0419] rac-diphenylsilylene-bis{1-(2-methyl,5-isopropylindenyl)}zirconium dichloride,

[0420] rac-methylphenylsilylene-bis{1-(2,5-dimethylindenyl)}zirconiumdichloride,

[0421] rac-methylphenylsilylene-bis{1-(2-methyl,5-isopropylindenyl)}zirconium dichloride,

[0422] rac-ethylene-bis{1-(2,6-dimethylindenyl)}zirconium dichloride,

[0423] rac-ethylene-bis{1-(2-methyl, 6-isopropylindenyl)}zirconiumdichloride,

[0424] rac-dimethylsilylene-bis{1-(2,6-dimethylindenyl)}zirconiumdichloride,

[0425] rac-dimethylsilylene-bis{1-(2-methyl,6-isopropylindenyl)}zirconium dichloride,

[0426] rac-diphenylsilylene-bis{1-(2,6-dimethylindenyl)}zirconiumdichloride,

[0427] rac-diphenylsilylene-bis{1-(2-methyl,6-isopropylindenyl)}zirconium dichloride,

[0428] rac-methylphenylsilylene-bis{1-(2,6-dimethylindenyl)}zirconiumdichloride,

[0429] rac-methylphenylsilylene-bis{1-(2-methyl,6-isopropylindenyl)}zirconium dichloride,

[0430] rac-ethylene-bis{1-(2,4,5-trimethylindenyl)}zirconium dichloride,

[0431] rac-ethylene-bis{1-(2-isopropyl-4,5-dimethylindenyl)}zirconiumdichloride,

[0432] rac-dimethylsilylene-bis{1-(2,4,5-trimethylindenyl)}zirconiumdichloride,

[0433] rac-diphenylsilylene-bis{1-(2,4,5-trimethylindenyl)}zirconiumdichloride,

[0434] rac-methylphenylsilylene-bis{1-(2,4,5-trimethylindenyl)}zirconiumdichloride,

[0435] rac-ethylene-bis{1-(2,5,6-trimethylindenyl)}zirconium dichloride,

[0436] rac-dimethylsilylene-bis{1-(2,5,6-trimethylindenyl)}zirconiumdichloride,

[0437] rac-diphenylsilylene-bis{1-(2,5,6-trimethylindenyl)}zirconiumdichloride,

[0438] rac-methylphenylsilylene-bis{1-(2,5,6-trimethylindenyl)}zirconiumdichloride,

[0439] rac-ethylene-bis{1-(2-methyl-5-t-butylindenyl)}zirconiumdichloride,

[0440] rac-dimethylsilyiene-bis{1-(2-methyl-5-t-butylindenyl)}zirconiumdichloride,

[0441] rac-diphenylsilylene-bis{-(2-methyl-5-t- butylindenyl)}zirconiumdichloride,

[0442]rac-methylphenylsilylene-bis{1-(2-methyl-5-t-butylindenyl)}zirconiumdichloride,

[0443] rac-ethylene-bis{1-(2-methyl-6-t-butylindenyl)}zirconiumdichloride,

[0444] rac-dimethylsilylene-bis{1-(2-methyl-6-t-butylindenyl)}zirconiumdichloride,

[0445] rac-diphenylsilylene-bis{1-(2-methyl-6-t-butylindenyl)}zirconiumdichloride,

[0446]rac-methylphenylsilylene-bis{1-(2-methyl-6-t-butylindenyl)}zirconiumdichloride,

[0447] rac-ethylene-bis{1-(2-methyl-5,6-di-t-butylindenyl)}zirconiumdichloride,

[0448]rac-dimethylsilylene-bis{1-(2-methyl-5,6-di-t-butylindenyl)}zirconiumdichloride,

[0449]rac-diphenylsilylene-bis{1-(2-methyl-5,6-di-t-butylindenyl)}zirconiumdichloride,

[0450]rac-methylphenylsilylene-bis{1-(2-methyl-5,6-di-t-butylindenyl)}zirconiumdichloride,

[0451] rac-ethylene-bis{1-(2-methyl-5-trimethylsilylindenyl)}zirconiumdichloride,

[0452]rac-dimethylsilylene-bis{1-(2-methyl-5-trimethylsilylindenyl)}zirconiumdichloride,

[0453]rac-diphenylsilylene-bis{1-(2-methyl-5-trimethylsilylindenyl)}zirconiumdichloride,

[0454]rac-methylphenylsilylene-bis{1-(2-methyl-5-trimethylsilylindenyl)}zirconiumdichloride,

[0455] rac-ethylene-bis{1-(2-methyl-6-trimethylsilylindenyl)}zirconiumdichloride,

[0456]rac-dimethylsilylene-bis{1-(2-methyl-6-trimethylsilylindenyl)}zirconiumdichloride,

[0457]rac-diphenylsilylene-bis{1-(2-methyl-6-trimethylsilylindenyl)}zirconiumdichloride,

[0458]rac-methylphenylsilylene-bis{1-(2-methyl-6-trimethylsilylindenyl)}zirconiumdichloride,

[0459]rac-ethylene-bis{1-(2-methyl-5,6-bistrimethylsilylindenyl)}zirconiumdichloride,

[0460]rac-dimethylsilylene-bis{1-(2-methyl-5,6-bistrimethylsilylindenyl)}zirconiumdichloride,

[0461]rac-diphenylsilylene-bis{1-(2-methyl-5,6-bistrimethylsilylindenyl)}zirconiumdichloride,

[0462]rac-methylphenylsilylene-bis{1-(2-methyl-5,6-bistrimethylsilylindenyl)}zirconiumdichloride,

[0463]rac-ethylene-bis{1-(2-methyl-5,6-bistriphenylsilylindenyl)}zirconiumdichloride,

[0464]rac-dimethylsilylene-bis{1-(2-methyl-5,6-bistriphenylsilylindenyl)}zirconium-dichloride,

[0465] rac-ethylene-bis{1-(2-methyl-4-methoxyindenyl)}zirconiumdichloride,

[0466] rac-dimethylsilylene-bis{1-(2-methyl-4-methoxyindenyl)}zirconiumdichloride,

[0467] rac-diphenylsilylene-bis{1-(2-methyl-4-methoxyindenyl)}zirconiumdichloride,

[0468]rac-methylphenylsilylene-bis{1-(2-methyl-4-methoxyindenyl)}zirconiumdichloride,

[0469] rac-dimethylsilylene-bis{1-(2-methyl-S-methoxyindenyl)}zirconiumdichloride,

[0470] rac-dimethylsilylene-bis{1-(2-methyl-6-methoxyindenyl)}zirconiumdichloride,

[0471] rac-ethylene-bis{1-(2-methyl-5,6-dimethoxyindenyl)}zirconiumdichloride,

[0472] ethylene-bis{1-(2-methyl-4,5,6,7-tetrahydroindenyl)}zirconiumdichloride,

[0473] dimethylsilylene-bis{1-(4,5,6,7-tetrahydroindenyl)}zirconiumdichloride,

[0474]dimethylsilylene-bis{1-(2-methyl-4,5,6,7-tetrahydroindenyl)}zirconiumdichloride,

[0475] dimethylsilylene-bis{1-(2-methylcyclopentadienyl)}zirconiumdichloride,

[0476] dimethylsilylene-bis{1-(3-methylcyclopentadienyl)}zirconiumdichloride,

[0477] dimethylsilylene-bis{1-(4-methylcyclopentadienyl)}zirconiumdichloride,

[0478] dimethylsilylene-bis{1-(5-methylcyclopentadienyl)}zirconiumdichloride,

[0479] dimethylsilylene-bis{1-(2,4-dimethylcyclopentadienyl)}zirconiumdichloride,

[0480] dimethylsilylene-bis{1-(2,5-dimethylcyclopentadienyl)}zirconiumdichloride,

[0481]dimethylsilylene-bis{1-(2,4,5-trimethylcyclopentadienyl)}zirconiumdichloride,

dimethylsilylene- bis(benzo[e]indenyl) zirconium dichloride

dimethylsilylene-bis(1,2- dihydroacenaphthylo[4,5- b]cyclopentadienyl)zirconium dichloride

dimethylsilylene-bis(7,8- dihydro-3H,6H-3-as- indathenyl)zirconiumdichloride

dimethylsilylene- bis(benzo[f]indenyl) zirconium dichloride

dimethylsilylene-bis{1- (toluo[4,3-f]-2-methyl-4-phenylindenyl)}zirconium dichloride

dimethylsilylene-bis{1- (benzo[f]-2-methyl-4- neopentylindenyl)zirconiumdichloride

[0482] There may also be used the compounds obtained by substitutingtitanium, hafnium, vanadium, niobium, tantalum or chromium for zirconiumin the above-exemplified zirconium compounds.

[0483] Of the transition metal compounds represented by the aforesaidformula (Ia), preferred are those having zirconium as the central metalatom and having at least two ligands containing an indenyl skeleton.

[0484] In the present invention, transition metal compounds preferablyused as the transition metal compound (a) are those represented by thefollowing formula (I):

[0485] wherein M is a transition metal atom of Group IVa, Group Va andGroup VIa of the periodic table. Examples the transition metal atomsinclude titanium, zirconium, hafnium, vanadium, niobium, tantalum,chromium, molybdenum and tungsten. Of these, preferred are titanium,zirconium and hafnium, and particularly preferred is zirconium.

[0486] R¹ is a hydrocarbon group of 2 to 6 carbon atoms. Examples of thehydrocarbon groups include an alkyl group such as ethyl, n-propyl,isopropyl, n-butyl, isobutyl, sec-butyl, tert-butyl, n-pentyl,neopentyl, n-hexyl and cyclohexyl; and an alkenyl group such as vinyland propenyl.

[0487] Of these, preferred are alkyl groups whose carbon bonded to theindenyl group is primary carbon, more preferred are alkyl groups of 2 to4 carbon atoms whose carbon bonded to the indenyl group is primarycarbon, and particularly preferred is ethyl.

[0488] R² is an aryl group of 6 to 16 carbon atoms. Examples of the arylgroups include phenyl, α-naphthyl, β-naphthyl, anthracenyl, phenanthryl,pyrenyl, acenaphthyl, phenarenyl, aceanthryrenyl, tetrahydronaphthyl andindanyl. Of these, preferred are phenyl, naphthyl, anthracenyl andphenanthryl.

[0489] These aryl groups may be substituted with:

[0490] halogen atoms, such as fluorine, chlorine, bromine and iodine;

[0491] hydrocarbon groups of 1 to 20 carbon atoms, such as alkyl groups(e.g., methyl, ethyl, propyl, butyl, hexyl cyclohexyl, octyl, nonyl,dodecyl, icosyl, norbornyl and adamantyl), alkenyl groups (e.g., vinyl,propenyl and cyclohexenyl), arylalkyl groups (e.g., benzyl, phenylethyland phenylpropyl) and aryl groups (e.g., phenyl, tolyl, dimethylphenyl,trimethylphenyl, ethylphenyl, propylphenyl, biphenyl, naphthyl,methylnaphthyl, anthracenyl and phenanthryl); and

[0492] organosilyl groups, such as trimethylsilyl, triethylsilyl andtriphenylsilyl.

[0493] X¹ and X² are each a hydrogen atom, a halogen atom, a hydrocarbongroup of 1 to 20 carbon atoms, a halogenated hydrocarbon group of 1 to20 carbon atoms, an oxygen-containing group or a sulfur-containinggroup. As the halogen atom and the hydrocarbon group of 1 to 20 carbonatoms, the aforesaid atoms and groups can be exemplified. As thehalogenated hydrocarbon group of 1 to 20 carbon atoms, groups obtainedby substituting the aforesaid hydrocarbon groups with halogen atoms canbe exemplified.

[0494] Examples of the oxygen-containing groups include hydroxy group;alkoxy groups such as methoxy, ethoxy, propoxy and butoxy; aryloxygroups such as phenoxy, methylphenoxy, dimethylphenoxy and naphthoxy;and arylalkoxy groups such as phenylmethoxy and phenylethoxy.

[0495] Examples of the sulfur-containing groups include substituentsobtained by substituting sulfur for oxygen in the above-mentionedoxygen-containing groups; sulfonate groups such as methylsulfonate,trifluoromethanesulfonate, phenylsulfonate, benzylsulfonate,p-toluenesulfonate, trimethylbenzenesulfonate,triisobutylbenzenesulfohate, p-chlorobenzenesulfonate andpentafluorobenzenesulfonate; and sulfinate groups such asmethylsulfinate, phenylsulfinate, benzenesulfonate, p-toluenesulfinate,trimehtylbenzenesulfinate and pentafluorobenzenesulfinate.

[0496] Of these, preferred are halogen atoms and hydrocarbon groups of 1to 20 carbon atoms.

[0497] Y is a divalent hydrocarbon group of 1 to 20 carbon atoms, adivalent halogenated hydrocarbon group of 1 to 20 carbon atoms, adivalent silicon-containing group, a divalent germanium-containinggroup, a divalent tin-containing group, —O—, —CO—, —S—, —SO—, —SO₂—,—NR³—, —P(R³)—, —P(O) (R³)—, —BR³—or —AlR³— (R³ is a hydrogen atom, ahalogen atom, a hydrocarbon group of 1 to 20 carbon atoms or ahalogenated hydrocarbon group of 1 to 20 carbon atoms). Morespecifically, there can be mentioned:

[0498] divalent hydrocarbon groups of 1 to 20 carbon atoms, such asalkylene groups, e.g., methylene, dimethylmethylene, 1,2-ethylene,dimethyl-1,2-ethylene, 1,3-trimethylene, 1,4-tetramethylene and1,2-cyclohexylene, 1,4-cyclohexylene, and arylalkylene groups, e.g.,diphenylmethylene and diphenyl-1,2-ethylene;

[0499] halogenated hydrocarbon groups obtained by halogenating theabove-mentioned divalent hydrocarbon groups of 1 to 20 carbon atoms,such as chloromethylene;

[0500] divalent silicon-containing groups, such as alkylsilylene,alkylatylsilylene and arylsilylene groups, e.g., methylsilylene,dimethylsilylene, diethylsilylene, di(n-propyl)silylene,di(i-propyl)silylene, di(cyclohexyl)silylene, methylphenylsilylene,diphenylsilylene, di(p-tolyl)silylene and di(p-chlorophenyl)silylene,and alkyldisilyl, alkylaryldisilyl and aryldisilyl groups, e.g.,tetramethyl-1,2-disilyl and tetraphenyl-1,2-disilyl;

[0501] divalent germanium-containing groups obtained by substitutinggermanium for silicon in the above-mentioned divalent silicon-containinggroups; and

[0502] divalent tin-containing groups obtained by substituting tin forsilicon in the above-mentioned divalent silicon-containing groups.

[0503] R³ is the same halogen atom, the same hydrocarbon group of 1 to20 carbon atoms or the same halogenated hydrocarbon group of 1 to 20carbon atoms as described above.

[0504] Of these, preferred are divalent silicon-containing groups,divalent germanium-containing groups and divalent tin-containing groups;more preferred are divalent silicon-containing groups; and mostpreferred are alkylsilylene, alkylarylsilylene and arylsilylene.

[0505] Exemplified below are the transition metal compounds representedby the above formula (I).

[0506] rac-dimethylsilylene-bis{1-(2-ethyl-4-phenylindenyl)}zirconiumdichloride,rac-dimethylsilylene-bis{1-(2-ethyl-4-α-naphthyl)indenyl)}zirconiumdichloride,

[0507]rac-dimethylsilylene-bis{1-(2-ethyl-4-(β-naphthyl)indenyl)}zirconiumdichloride,

[0508]rac-dimethylsilylene-bis{1-(2-etlhyl-4-(2-methyl-1-naphthyl)indenyl)}zirconiumdichloride,

[0509]rac-dimethylsilylene-bis{1-(2-ethyl-4-(5-acenaphthyl)indenyl)}zirconiumdichloride,

[0510]rac-dimethylsilylene-bis{1-(2-ethyl-4-(9-anthracenyl)indenyl)}zirconiumdichloride,

[0511]rac-dimethylsilylene-bis{1-(2-ethyl-4-(9-phenantoryl)indenyl)}zirconiumdichloride,

[0512]rac-dimethylsilylene-bis{1-(2-ethyl-4-(o-methylphenyl)indenyl)}zirconiumdichloride,

[0513]rac-dimethylsilylene-bis{1-(2-ethyl-4-(m-methylphenyl)indenyl)}zirconiumdichloride,

[0514]rac-dimethylsilylene-bis{1-(2-ethyl-4-(p-methylphenyl)indenyl)}zirconiumdichloride,

[0515]rac-dimethylsilylene-bis{1-(2-ethyl-4-(2,3-dimethylphenyl)indenyl)}zirconiumdichloride,

[0516]rac-dimethylsilylene-bis{1-(2-ethyl-4-(2,4-dimethylphenyl)indenyl)}zirconiumdichloride,

[0517]rac-dimethylsilylene-bis{1-(2-ethyl-4-(2,5-dimethylphenyl)indenyl)}zirconiumdichloride,

[0518]rac-dimethylsilylene-bis{1-(2-ethyl-4-(2,4,6-trimethylphenyl)indenyl)}zirconiumdichloride,

[0519]rac-dimethylsilylene-bis{1-(2-ethyl-4-(o-chlorophenyl)indenyl)}zirconiumdichloride,

[0520]rac-dimethylsilylene-bis{1-(2-ethyl-4-(m-chlorophenyl)indenyl)}zirconiumdichloride,

[0521]rac-dimethylsilylene-bis{1-(2-ethyl-4-(p-chlorophenyl)indenyl)}zirconiumdichloride,

[0522]rac-dimethylsilylene-bis{1-(2-ethyl-4-(2,3-dichlorophenyl)indenyl)}zirconiumdichloride,

[0523]rac-dimethylsilylene-bis{1-(2-ethyl-4-(2,6-dichlorophenyl)indenyl)}zirconiumdichloride,

[0524]rac-dimethylsilylene-bis{1-(2-ethyl-4-(3,5-dichlorophenyl)-indenyl)}zirconiumdichloride,

[0525]rac-dimethylsilylene-bis{1-(2-ethyl-4-(2-bromophenyl)indenyl)}zirconiumdichloride,

[0526]rac-dimethylsilylene-bis{1-(2-ethyl-4-(3-bromophenyl)indenyl)}zirconiumdichloride,

[0527]rac-dimethylsilylene-bis{1-(2-ethyl-4-(4-bromophenyl)indenyl)}zirconiumdichloride,

[0528]rac-dimethylsilylene-bis{1-(2-ethyl-4-(4-biphenylyl)indenyl)}zirconiumdichloride,

[0529]rac-dimethylsilylene-bis{1-(2-ethyl-4-(4-trimethylsilylphenyl)indenyl)}zirconiumdichloride,

[0530] rac-dimethylsilylene-bis{1-(2-n-propyl-4-phenylindenyl)}zirconiumdichloride,

[0531]rac-dimethylsilylene-bis{1-(2-n-propyl-4-[(α-naphthyl)indenyl)}zirconiumdichloride,

[0532]rac-dimethylsilylene-bis{1-(2-n-propyl-4-(β-naphthyl)indenyl)}zirconiumdichloride,

[0533]rac-dimethylsilylene-bis{1-(2-n-propyl-4-(2-methyl-1-naphthyl)indenyl)}zirconiumdichloride,

[0534] rac-dimethylsilylene-bis{1-(2-n-propyl-4-(5-acenaphthyl)indenyl)}zirconium dichloride,

[0535]rac-dimethylsilylene-bis{1-(2-n-propyl-4-(9-anthracenyl)indenyl)}zirconiumdichloride,

[0536]rac-dimethylsilylene-bis{1-(2-n-propyl-4-(9-phenantoryl)indenyl)}zirconiumdichloride,

[0537] rac-dimethylsilylene-bis{1-(2-1-propyl-4-phenylindenyl)}zirconiumdichloride,

[0538]rac-dimethylsilylene-bis{1-(2-1-propyl-4-α-naphthyl)indenyl)}zirconiumdichloride,

[0539]rac-dimethylsilylene-bis{1-(2-1-propyl-4-(β-naphthyl)indenyl)}zirconiumdichloride,

[0540]rac-dimethylsilylene-bis{1-(2-1-propyl-4-(2-methyl-1-naphthyl)indenyl)}zirconiumdichloride,

[0541]rac-dimethylsilylene-bis{1-(2-1-propyl-4-(5-acenaphthyl)indenyl)}zirconiumdichloride,

[0542]rac-dimethylsilylene-bis{1-(2-1-propyl-4-(9-anthracenyl)indenyl)}zirconiumdichloride,

[0543]rac-dimethylsilylene-bis{1-(2-1-propyl-4-(9-phenantoryl)indenyl)}zirconiumdichloride,

[0544] rac-dimethylsilylene-bis{1-(2-s-butyl-4-phenylindenyl)}zirconiumdichloride,

[0545]rac-dimethylsilylene-bis{1-(2-s-butyl-4-α-naphthyl)indenyl)}zirconiumdichloride,

[0546]rac-dimethylsilylene-bis{1-(2-s-butyl-4-(β-naphthyl)indenyl)}zirconiumdichloride,

[0547]rac-dimethylsilylene-bis{1-(2-s-butyl-4-(8-methyl-9-naphthyl)indenyl)}zirconiumdichloride,

[0548]rac-dimethylsilylene-bis{1-(2-s-butyl-4-(5-acenaphthyl)indenyl)}zirconiumdichloride,

[0549]rac-dimethylsilylene-bis{1-(2-s-butyl-4-(9-anthracenyl)indenyl)}zirconiumdichloride,

[0550]rac-dimethylsilylene-bis{1-(2-s-butyl-4-(9-phenantoryl)indenyl)}zirconiumdichloride,

[0551] rac-dimethylsilylene-bis{1-(2-n-pentyl-4-phenylindenyl)}zirconiumdichloride,

[0552]rac-dimethylsilylene-bis{1-(2-n-pentyl-4-(α-naphthyl)indenyl)}zirconiumdichloride,

[0553] rac-dimethylsilylene-bis{1-(2-n-butyl-4-phenylindenyl)}zirconiumdichloride,

[0554]rac-dimethylsilylene-bis{1-(2-n-butyl-4-(α-naphthyl)indenyl)}zirconiumdichloride,

[0555]rac-dimethylsilylene-bis{1-(2-n-butyl-4-(β-naphthyl)indenyl)}zirconiumdichloride,

[0556]rac-dimethylsilylene-bis{1-(2-n-butyl-4-(2-methyl-1-naphthyl)indenyl)}zirconiumdichloride,

[0557]rac-dimethylsilylene-bis{1-(2-n-butyl-4-(5-acenaphthyl)indenyl)}zirconiumdichloride,

[0558]rac-dimethylsilylene-bis{1-(2-n-butyl-4-(9-anthracenyl)indenyl)}zirconiumdichloride,

[0559]rac-dimethlsilylene-bis{1-(2-n-butyl-4-(9-phenantoryl)indenyl)}zirconiumdichloride,

[0560] rac-dimethylsilylene-bis{1-(2-1-butyl-4-phenylindenyl)}zirconiumdichloride,

[0561]rac-dimethylsilylene-bis{1-(2-1-butyl-4-(α-naphthyl)indenyl)}zirconiumdichloride,

[0562]rac-dimethylsilylene-bis{1-(2-1-butyl-4-(β-naphthyl)indenyl)}zirconiumdichloride,

[0563]rac-dimethylsilylene-bis{1-(2-1-butyl-4-(2-methyl-1-naphthyl)indenyl)}zirconiumdichloride,

[0564]rac-dimethylsilylene-bis{1-(2-1-butyl-4-(5-acenaphthyl)indenyl)}zirconiumdichloride,

[0565]rac-dimethylsilylene-bis{1-(2-1-butyl-4-(9-anthracenyl)indenyl)}zirconiumdichloride,

[0566]rac-dimethylsilylene-bis{1-(2-1-butyl-4-(9-phenantoryl)indenyl)}zirconiumdichloride,

[0567]rac-dimethylsilylene-bis{1-(2-neopentyl-4-phenylindenyl)}zirconiumdichloride,

[0568]rac-dimethylsilylene-bis{1-(2-neopentyl-4-α-naphthyl)indenyl)}zirconiumdichloride,

[0569] rac-dimethylsilylene-bis{1-(2-n-hexyl-4-phenylindenyl)}zirconiumdichloride,

[0570]rac-dimethylsilylene-bis{1-(2-n-hexyl-4-[(α-naphthyl)indenyl)}zirconiumdichloride,

[0571]rac-methylphenylsilylene-bis{1-(2-ethyl-4-phenylindenyl)}zirconiumdichloride,

[0572]rac-methylphenylsilylene-bis{1-(2-ethyl-4-α-naphthyl)indenyl)}zirconiumdichloride,

[0573]rac-methylphenylsilylene-bis{1-(2-ethyl-1-4-(9-anthracenyl)indenyl)}zirconiumdichloride,

[0574]rac-methylphenylsilylene-bis{1-(2-ethyl-4-(9-phenantoryl)indenyl)}zirconiumdichloride,

[0575] rac-diphenylsilylene-bis{1-(2-ethyl-4-phenylindenyl)}zirconiumdichloride,

[0576]rac-diphenylsilylene-bis{1-(2-ethyl-4-α-naphthyl)indenyl)}zirconiumdichloride,

[0577]rac-diphenylsilylene-bis{1-(2-ethyl-4-(9-anthracenyl)indenyl)}zirconiumdichloride,

[0578]rac-diphenylsilylene-bis{1-(2-eth-yl-4-(9-phenantoryl)indenyl)}zirconiumdichloride,

[0579]rac-diphenylsilylene-bis{1-(2-ethyl-4-(4-biphenyl)indenyl)}zirconiumdichloride,

[0580] rac-methylene-bis{1-(2-ethyl-4-phenylindenyl)}zirconiumdichloride,

[0581] rac-methylene-bis{1-(2-ethyl-4-α-naphthyl)indenyl)}zirconiumdichloride,

[0582] rac-ethylene-bis{1-(2-ethyl-4-phenylindenyl)}zirconiumdichloride,

[0583] rac-ethylene-bis{1-(2-ethyl-4-(α-naphthyl)indenyl)}zirconiumdichloride,

[0584] rac-ethylene-bis{1-(2-n-propyl-4-α-naphthyl)indenyl)}zirconiumdichloride,

[0585] rac-dimethylgermyl-bis{1-(2-ethyl-4-phenylindenyl)}zirconiumdichloride,

[0586]rac-dimethylgermyl-bis{1-(2-ethyl-4-(α-naphthyl)indenyl)}zirconiumdichloride, and

[0587] rac-dimethylgermyl-bis{1-(2-n-propyl-4-phenylindenyl)}zirconiumdichloride.

[0588] There may also be used the transition metal compounds obtained bysubstituting titanium metal, hafnium metal, vanadium metal, niobiummetal, tantalum metal, chromium metal, molybdenum metal or tungstenmetal for zirconium metal in the above-exemplified compounds.

[0589] The transition metal compounds represented by the above formula(I) can be prepared in accordance with the methods described in Journalof Organometallic Chem. 288 (1985), pages 63 to 67, European PatentPublication No. 0,320,762 specification and Examples thereof, forinstance, by the following manner.

[0590] wherein, Z represents Cl, Br, I or o-tosyl group, and H₂R^(a)represents

[0591] Though the transition metal compounds represented by theaformentioned formula (I) are usually used in the form of racemicmodification, R-type or S-type may also be used.

[0592] These transition metal compounds may be used singly or incombination of two or more kinds. Further, they may be diluted inhydrocarbon or halogenated hydrocarbon.

[0593] The organoaluminum oxy-compound which forms the olefinpolymerization catalyst (1) for polymerization of the propylene polymer(A1) and the propylene polymer (2) may be a known benzene-solublealuminoxane or the benzene-insoluble organoaluminum oxy-compound havingbeen disclosed in JP-A-2-78687/1990.

[0594] The above-mentioned known aluminoxane may be prepared, forexample, by the following procedures:

[0595] (1) a procedure for recovering an aluminoxane as its hydrocarbonsolution which comprises adding an organoaluminum compound such astrialkylaluminum to a suspension in a hydrocarbon medium of a compoundcontaining adsorbed water, or a salt containing water of crystallizationsuch as magnesium chloride hydrate, copper sulfate hydrate, aluminumsulfate hydrate, nickel sulfate hydrate and cerium chloride hydrate, andreacting the organoaluminum compound;

[0596] (2) a procedure for recovering an aluminoxane as its hydrocarbonsolution which comprises reacting water, ice or steam directly with anorganoaluminum compound such as trialkylaluminum in a solvent such asbenzene, toluene, ethyl ether and tetrahydrofuran; and

[0597] (3) a procedure for recovering an aluminoxane which comprisesreacting an organotinoxide such as dimethyltinoxide and dibutyltinoxidewith an organoaluminum compound such as trialkylaluminum in a solventsuch as decane, benzene or toluene.

[0598] Moreover, the aluminoxane may contain a small amount of anorganometal component. Furthermore, the solvent or unreactedorganoaluminum compound may be removed from the above-mentionedrecovered aluminoxane-containing solution, by distillation, and thealuminoxane may be redissolved in a solvent.

[0599] Concrete examples of the organoaluminum compound used for thepreparation of the aluminoxane include

[0600] trialkylaluminum such as trimethylaluminum, triethylaluminum,tripropylaluminum, triisopropylaluminum, tri-n-butylaluminum,triisobutylaluminum, tri-sec-butylaluminum, tri-tert-butylaluminum,tripentylaluminum, trihexylaluminum, trioctylaluminum andtridecylaluminum;

[0601] tricycloalkylaluminums such as tricyclohexylaluminum andtricyclooctylaluminum;

[0602] dialkylaluminum halides such as dimethylaluminum chloride,diethylaluminum chloride, diethylaluminum bromide and diisobutylaluminumchloride;

[0603] dialkylaluminum hydrides such as diethylaluminum hydride anddiisobutylaluminum hydride;

[0604] dialkylaluminum alkoxides such as dimethylaluminum methoxide anddiethylaluminum ethoxide; and

[0605] dialkylaluminum aryloxides such as diethylaluminum phenoxide.

[0606] Of these compounds, trialkylaluminum and tricyclo-alkylaluminumare preferable, and trimethylaluminum is particularly preferable.

[0607] Furthermore, there may also be used as the organoaluminumcompound isoprenylaluminum represented by the general formula

(i-C₄H₉)_(x)Al_(y)(C₅H₁₀)_(z)

[0608] wherein x, y and z are each a positive number, and z≧2x.

[0609] The organoaluminum compounds mentioned above may be used eithersingly or in combination.

[0610] Solvents used for the solutions of the aluminoxane includearomatic hydrocarbons such as benzene, toluene, xylene, cumene andcymene; aliphatic hydrocarbons such as pentane, hexane-, heptane,octane, decane, dodecane, hexadecane and octadecane; alicyclichydrocarbons such as cyclopentane, cyclohexane, cyclooctane andmethylcyclopentane; petroleum fractions such as gasoline, kerosene andgas oil; and halogenated compounds derived from the above-mentionedaromatic hydrocarbons, aliphatic hydrocarbons and alicyclichydrocarbons, especially chlorinated and brominated hydrocarbons. Inaddition, there may also be used ethers such as ethyl ether andtetrahydrofuran. Of these solvents as exemplified above, aromatichydrocarbons or aliphatic hydrocarbons are particularly preferred.

[0611] As the compound (c) which reacts with the aforesaid transitionmetal compound (a) to form an ion pair and which is used for forming theolefin polymerization catalyst (1) employable for the preparation of thepropylene polymer (Al) and the propylene polymer (A2), there can bementioned Lewis acid, ionic compounds and carborane compounds describedin JP-A-1-501950/1989, JP-A-1-502036/1989, JP-A-3-179005/1992,JP-A-3-179006/1992, JP-A-0.3-207703/1992 and JP-A-3-207704/1992, andU.S. Patent Application No. 547718 (now U.S. Pat. No. 5,321,106).

[0612] Examples of the Lewis acid include triphenylboron,tris(4-fluorophenyl)boron, tris(p-tolyl)boron, tris(o-tolyl)boron,tris(3,5-dimethylphenyl)boron, tris(pentafluorophenyl)boron, MgCl₂,Al₂O₃ and SiO₂-Al₂O₃.

[0613] Examples of the ionic compounds includetriphenylcarbeniumtetrakis(pentafluorophenyl)borate,tri-n-butylammoniumtetrakis(pentafluorophenyl)borate,N,N-dimethylaniliniumtetrakis(pentafluorophenyl)borate andferroceniumtetra(pentafluorophenyl)borate.

[0614] Examples of the carborane compounds include dodecaborane,1-carbaundacaborane, bis-n-butylammonium(1-carbedodeca)borate,tri-n-butylammonium(7,8-dicarbaundeca)borate andtri-n-butylammonium(tridecahydride-7-carbaundeca)borate.

[0615] The compound (c) which reacts with the transition metal compound(a) to form an ion pair can be used in combination of two or more kinds.

[0616] The olefin polymerization catalyst (1) used for preparing thepropylene polymer (A1) and the propylene polymer (A2) is formed from thetransition metal compound (a) and at least one compound selected fromthe organoaluminum oxy-compound (b) and the compound (c). However, thecatalyst (1) may further contain an organoaluminum compound (j), ifnecessary, together with the above components.

[0617] The organoaluminum compound (j) is, for example, anorganoaluminum compound represented by the following formula (II):

R ⁹ _(n)AlX_(3-n)  (II)

[0618] wherein R⁹ is a hydrocarbon group of 1 to 12 carbon atoms, X is ahalogen atom, and n is 1 to 3.

[0619] In the above formula (II), R⁹ is a hydrocarbon group of 1 to 12carbon atoms, for example, an alkyl group, a cycloalkyl group or an arylgroup. Examples of those groups include methyl, ethyl, n-propyl,isopropyl, isobutyl, pentyl, hexyl, octyl, cyclopentyl, cyclohexyl,phenyl and tolyl.

[0620] Particular examples of such organoaluminum compounds (j) include:

[0621] trialkylaluminums, such as trimethylaluminum, triethylaluminum,triisopropylaluminum, triisobutylaluminum, trioctylaluminum,tri(2-ethylhexyl)aluminum and tridecylaluminum;

[0622] alkenylaluminums, such as isoprenylaluminum;

[0623] dialkylaluminum halides, such as dimethylaluminum chloride,diethylaluminum chloride, diisopropylaluminum chloride,diisobutylaluminum chloride and dimethylaluminum bromide;

[0624] alkylaluminum sesquihalides, such as methylaluminumsesquichloride, ethylaluminum sesquichloride, isopropylaluminumsesquichloride, butylaluminum sesquichloride and ethylaluminumsesquibromide;

[0625] alkylaluminum dihalides, such as methylaluminum dichloride,ethylaluminum dichloride, isopropylaluminum dichloride and ethylaluminumdibromide; and alkylaluminum hydrides, such as diethylaluminum hydrideand diisobutylaluminum hydride.

[0626] Also employable as the organoaluminum compound (j) is a compoundrepresented by the following formula (III):

R⁹AlL_(3-n)  (III)

[0627] wherein R⁹ is the same as above, L is —OR¹⁰ group, —OSiR¹¹ ₃group, —OAlR¹² ₂ group, —NR¹³ ₂ group, —SiR¹⁴ ₃ group or —N(R¹⁵)AlR¹⁶ ₂group; n is 1 or 2; R¹⁰, R¹¹, R¹² and R¹⁶ are each methyl, ethyl,isopropyl, isobutyl, cyclohexyl, phenyl or the like; R¹³ is a hydrogenatom, methyl, ethyl, isopropyl, phenyl, trimethylsilyl or the like; andR¹⁴ and R¹⁵ are each methyl, ethyl or the like.

[0628] Of such organoaluminum compounds, preferred are compoundsrepresented by the formula R⁹ _(n)Al(OAlR¹⁰ ₂)_(3-n), for example,Et₂AlOAlEt₂, and (iso-Bu)₂AlOAl (iso-Bu) 2.

[0629] Of the organoaluminum compounds represented by the above formulas(II) and (III), preferred are compounds represented by the formulaR⁹nAl, and particularly preferred are compounds of the formula R⁹ Alwherein R⁹ is an isoalkyl group.

[0630] The olefin polymerization catalyst (1) used for preparing thepropylene polymer (A1) and the propylene polymer (A2) can be prepared bymixing the transition metal compound (a) [component (a)] and theorganoaluminum oxy-compound (b) [component (b)] (or the compound (c)which reacts with the transition metal compound (a) to form an ion pair,(component (c)]), and if desired, the organoaluminum compound (j)(component (j)] in an inert hydrocarbon solvent or an olefin solvent.

[0631] Examples of the inert hydrocarbon solvents used for preparing theolefin polymerization catalyst (1) include:

[0632] aliphatic hydrocarbons, such as propane, butane, pentane, hexane,heptane, octane, decane, dodecane and kerosine;

[0633] alicyclic hydrocarbons, such as cyclopentane, cyclohexane andmethylcyclopentane;

[0634] aromatic hydrocarbons, such as benzene, toluene and xylene;

[0635] halogenated hydrocarbons, such as ethylene chloride,chlorobenzene and dichloromethane; and

[0636] mixtures of the above hydrocarbons.

[0637] In the preparation of the olefin polymerization catalyst (1),each components may be mixed in an optional order, but preferably theyare mixed in the following manner:

[0638] the component (b) [or the component (c)] is mixed with thecomponent (a);

[0639] the component (b) is mixed with the component (j), and theresulting mixture is then mixed with the component (a);

[0640] the component (a) is mixed with the component (b) [or thecomponent (c)], and the resulting mixture is then mixed with thecomponent (j); or

[0641] the component (a) is mixed with the component (j), and theresulting mixture is then mixed with the component (b) [or the component(c)].

[0642] In the mixing of each components, an atomic ratio (Al/transitionmetal) of the aluminum in the component (b) to the transition metal inthe component (a) is in the range of usually 10 to 10,000, preferably 20to 5,000; and a concentration of the component (a) is in the range ofabout 10⁻⁸ to 10⁻¹ mol/1-solvent, preferably 10⁻⁷ to 5×10-2mol/1-solvent.

[0643] When the component (c) is used, a molar ratio [component(a)/component (c)] of the component (a) to the component (c) is in therange of usually 0.01 to 10, preferably 0.1 to 5; and a concentration ofthe component (a) is in the range of about 10⁻⁸ to 10⁻¹ mol/1-solvent,preferably 10⁻⁷ to 5×10⁻² mol/1-solvent.

[0644] When the component (j) is used, an atomic ratio (Al_(j)/Al_(b))of the aluminum atom (Al_(j)) in the component (j) to the aluminum atom(Al_(b)) in the component (b) is in the range of usually 0.02 to 20,preferably 0.2 to 10.

[0645] The above-mentioned catalyst components may be mixed in apolymerizer. Otherwise, a mixture of the components beforehand preparedmay be fed to a polymerizer.

[0646] If the components are beforehand mixed, the mixing temperature isin the range of usually −50 to 150° C., preferably −20 to 120° C.; andthe contact time is in the range of 1 to 1,000 minutes, preferably 5 to600 minutes. The mixing temperature may be varied while the componentsare mixed and contacted with each other.

[0647] The olefin polymerization catalyst (1) may be an olefinpolymerization solid catalyst in which at least one of the component(a), the component (b) (or the component (c)) and the component (j) issupported on an inorganic or organic carrier of granular or particulatesolid.

[0648] The inorganic carrier is preferably a porous oxide, for example,SiO₂ or Al₂O₃.

[0649] Examples of the granular or particulate solid organic compoundsinclude polymers or copolymers produced mainly from α-olefins such asethylene, propylene and 1-butene or styrene.

[0650] The olefin polymerization catalyst (1) may be a prepolymerizedcatalyst for olefin polymerization formed from the particulate carrier,the component (a), the component (b) [or the component (c)] and anolefin polymer produced by the prepolymerization, and if desired, thecomponent (j).

[0651] The olefin used for the prepolymerization includes propylene,ethylene and 1-butene. Further, a mixture of these olefins and otherolefin may also be employed.

[0652] In addition to the above components, the olefin polymerizationcatalyst (1) may contain other components which are useful for theolefin polymerization, for example, water as a catalyst component.

[0653] The propylene polymer (A1) and the propylene polymer (A2) can beprepared by polymerizing propylene in the presence of the olefinpolymerization catalyst (1). In the polymerization of propylene,monomers such as ethylene and α-olefins of 4 to 20 carbon atoms (e.g.,1-butene, 1-pentene, 1-hexene, 4-methyl-1-pentene, 1-octene, 1-decene,1-dodecene, 1-tetradecene, 1-hexadecene, 1-octadecene and 1-eicosene)may be used in amounts of not more than 0.1 mol.

[0654] The polymerization may be carried out by either a liquid phasepolymerization process such as a suspension polymerization process and asolution polymerization process, or a gas phase polymerization process.

[0655] In the liquid phase polymerization process, the same inerthydrocarbon solvent as used in the preparation of the catalyst describedbefore can be used, or propylene can be also used as a solvent.

[0656] In the suspension polymerization process, the temperature forpolymerizing propylene is in the range of usually −50 to 100° C.,preferably 0 to 90° C. In the solution polymerization process, thepolymerization temperature is in the range of usually 0 to 250° C.,preferably 20 to 200° C. In the gas phase polymerization process, thepolymerization temperature is in the range of usually 0 to 120° C.,preferably 20 to 100° C. The polymerization pressure is in the range ofusually atmospheric pressure to 100 kg/cm², preferably atmosphericpressure to 50 kg/cm². The polymerization reaction may be carried outeither batchwise, semi-continuously or continuously. Further, it is alsopossible to conduct the polymerization in two or more steps havingdifferent reaction conditions.

[0657] The molecular weight of the resulting propylene polymer can beregulated by allowing hydrogen to exist in the polymerization system orby varying the polymerization temperature and the polymerizationpressure.

The Second Propylene Polymer Composition

[0658] The second propylene polymer composition comprises:

[0659] (Al) a propylene polymer which is characterized in that:

[0660] the propylene polymer is prepared by the use of an olefinpolymerization catalyst comprising:

[0661] (i) (a) a transition metal compound, and

[0662] (ii) at least one compound selected from the group consisting of

[0663] (b) an organoaluminum oxy-compound, and

[0664] (c) a compound which reacts with the transition metal compound(a) to form an ion pair,

[0665] the propylene polymer has a melt flow rate (MFR), as measured at230° C. under a load of 2.16 kg, of 0.01 to 30 g/10 min, and

[0666] the propylene polymer has a molecular weight distribution(Mw/Mn), as measured by GPC, of 2 to 3;

[0667] (A2) a propylene polymer which is characterized in that:

[0668] the propylene polymer is prepared by the use of an olefinpolymerization catalyst comprising:

[0669] (i) (a) a transition metal compound, and

[0670] (ii) at least one compound selected from the group consisting of

[0671] (b) an organoaluminum oxy-compound, and

[0672] (c) a compound which reacts with the transition metal compound(a) to form an ion pair,

[0673] the propylene polymer has a melt flow rate (MFR), as measured at230° C. under a load of 2.16 kg, of 30 to 1,000 g/10 min, and

[0674] the propylene polymer has a molecular weight distribution(Mw/Mn), as measured by GPC, of 2 to 4; and (B) a soft polymer.

[0675] In this propylene polymer composition, the ratio ((A2)/(A1)) ofthe MFR of said propylene polymer (A2) to the MFR of said propylenepolymer (A1) is not less than 30.

[0676] Propylene Polymer (Al)

[0677] The propylene polymer (A1) for constituting the second propylenepolymer composition is identical with the propylene polymer (A1) forconstituting the first propylene polymer composition.

[0678] Propylene Polymer (A2)

[0679] The propylene polymer (A²) for constituting the second propylenepolymer composition is identical with the propylene polymer (A2) forconstituting the first propylene polymer composition.

[0680] Soft Polymer (B)

[0681] The soft polymer (B) for constituting the second propylenepolymer composition is a (co)polymer of an α-olefin of 2 to 20 carbonatoms, and desirably has MFR, as measured at 190° C. under a load of2.16 kg, of 0.01 to 100 g/10 min, preferably 0.05 to 50 g/10 min. Thissoft polymer (B) has a crystallinity, as measured by X-raydiffractometry, of less than 30%, and desirably is amorphous.

[0682] Examples of the α-olefins of 2 to 20 carbon atoms includeethylene, propylene, 1-butene, 1-pentene, 1-hexene, 4-methyl-1-pentene,1-octene, 1-decene and mixtures thereof. Of these, particularlypreferred are α-olefins of 1 to 10 carbon atoms.

[0683] The soft polymer (B) is preferably a copolymer of ethylene and anα-olefin, and the α-olefin is for example an α-olefin of 3 to 20 carbonatoms, preferably an α-olefin of 3 to 6 carbon atoms, particularlypreferably propylene.

[0684] The soft polymer (B) may contain other constituent units than theconstituent units derived from α-olefins, such as those derived fromdiene compounds, with the proviso that the characteristics thereof arenot marred.

[0685] Examples of the constituent units which are allowed to becontained in the soft polymer (B) include constituent units derivedfrom:

[0686] chain non-conjugated dienes, such as 1,4-hexadiene,1,6-octadiene, 2-methyl-1,5-hexadiene, 6-methyl-1,5-heptadiene and7-methyl-1,6-octadiene;

[0687] cyclic non-conjugated dienes, such as cyclohexadiene,dicyclopentadiene, methyltetrahydroindene, 5-vinylnorbornene,5-ethylidene-2-norbornene, 5-methylene-2-norbornene,5-isopropylidene-2-norbornene and6-chloromethyl-5-isopropenyl-2-norbornene; and

[0688] diene compounds, such as 2,3-diisopropylidene-5-norbornene,2-ethylidene-3-isopropylidene-5-norbornene and2-propenyl-2,2-norbornadiene.

[0689] These diene components can be used singly or in combination. Acontent of the diene component is usually not more than 10% by mol,preferably 0 to 5% by mol.

[0690] The soft polymer (B) is, for example, a copolymer containingconstituent units derived from ethylene in an amount of 0 to 95% by mol,preferably 30 to 92% by mol, more preferably 40 to 90% by mol,constituent units derived from an α-olefin of 3 to 20 carbon atoms in anamount of 1 to 100% by mol, preferably 4 to 70% by mol, more preferably8 to 60% by mol, and constituent units derived from the diene componentin an amount of 0 to 10% by mol, preferably 0 to 5% by mol, morepreferably 0 to 3% by mol.

[0691] Such soft polymer (B) as mentioned above can be prepared byconventionally known processes using a titanium catalyst, a vanadiumcatalyst, a zirconium catalysts, etc.

[0692] Propylene Polymer Composition

[0693] The second propylene polymer composition comprises the propylenepolymer (A1), the propylene polymer (A2) and the soft polymer (B). Inthis composition, it is desired that the propylene polymer (A1) iscontained in an amount of 10 to 90 parts by weight, preferably 30 to 70parts by weight; the propylene polymer (A2) is contained in an amount of10 to 90 parts by weight, preferably 30 to 70 parts by weight; and thesoft polymer (B) is contained in an amount of 3 to 30 parts by weight,preferably 10 to 25 parts by weight. A ratio [(A2)/(A1)] of the MFR ofthe propylene polymer (A2) to the MFR of the propylene polymer (A1) isnot less than 30, preferably in the range of 40 to 300, more preferably50 to 100.

[0694] The second propylene polymer composition is desired to have MFR,as measured at 230° C. under a load of 2.16 kg, of 1 to 100 g/10 min,preferably 5 to 50 g/10 min. In this composition, Mw/Mn of all thepropylene components for constituting the composition is desirably inthe range of 4 to 15.

[0695] The density of the second propylene polymer composition isdesired to be in the range of 0.88 to 0.92 g/cm³, preferably 0.89 to0.92 g/cm³.

[0696] The heat distortion temperature (HDT) thereof is desired to benot lower than 80° C., preferably in the range of 90 to 140° C.

[0697] The flexural modulus (FM) thereof is desired to be in the rangeof 8,500 to 18,000 kg/cm², preferably 9,000 to 15,000 kg/cm².

[0698] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 10 to 50 kg·cm/cm, preferably 10 to 40 kg·cm/cm.

[0699] The tensile elongation at break (EL) thereof is desired to be inthe range of 200 to 1,000%, preferably 300 to 1,000%.

[0700] The second propylene polymer composition may contain, ifnecessary, additives which may be added to the first propylene polymercomposition, with the proviso that the object of the invention is notmarred.

[0701] The second propylene polymer composition can be prepared by knownprocesses. For example, the composition can be prepared in accordancewith the processes (1) to (5) described for the first propylene polymercomposition, using the propylene polymer (A1), the propylene polymer(A2), the soft polymer (B) and if desired other components which may beoptionally added.

[0702] The second propylene polymer composition may be prepared byforming a composition of the propylene polymer (A1) and the propylenepolymer (A2), which has been beforehand prepared in the followingmanner, and then blending the resulting composition with the softpolymer (B) in accordance with the aforesaid processes.

[0703] The composition of the propylene polymer (A1) and the propylenepolymer (A2) can be produced by a process comprising conducting thepolymerization in two or more steps having different reactionconditions, in one step of which the propylene polymer (A1) is preparedand in another step of which the propylene polymer (A2) is prepared, ora process comprising using-plural polymerizers, in one polymerizer ofwhich the propylene polymer (A1) is prepared and in another polymerizerof which the propylene polymer (A2) is prepared.

[0704] The second propylene polymer composition as mentioned above isexcellent in not only heat resistance, rigidity and tensile elongationat break but also moldability and impact resistance. Further, since theamount of the catalyst residue in the polymer composition is small, thearticle molded from the composition is never colored and is good insanitariness.

The Third Propylene Polymer Composition

[0705] The third propylene polymer composition comprises:

[0706] (A3) a propylene polymer which is prepared by the use of anolefin polymerization catalyst comprising (d) a solid titanium catalystcomponent and (e) an organometallic compound catalyst component, saidcomponents (d) and (e) being described later, and which has a melt flowrate (MFR), as measured at 230° C. under a load of 2.16 kg, of 0.01 to30 g/10 min, and a molecular weight distribution (Mw/Mn), as measured byGPC, of 4 to 15; and

[0707] (A2) a propylene polymer which is characterized in that:

[0708] the propylene polymer is prepared by the use of an olefinpolymerization catalyst comprising:

[0709] (i) (a) a transition metal compound, and

[0710] (ii) at least one compound selected from the group consisting of

[0711] (b) an organoaluminum oxy-compound, and

[0712] (c) a compound which reacts with the transition metal compound(a) to form an ion pair,

[0713] the propylene polymer has a melt flow rate (MFR), as measured at230° C. under a load of 2.16 kg, of 30 to 1,000 g/10 min, and

[0714] the propylene polymer has a molecular weight distribution(Mw/Mn), as measured by GPC, of 2 to 4.

[0715] Propylene Polymer (A3)

[0716] The propylene polymer (A3) for constituting the third propylenepolymer composition is a propylene homopolymer or a propylene copolymerobtained by the use of an olefin polymerization catalyst comprising asolid titanium catalyst component (d) and an organometallic compoundcatalyst component (e), both components being described later.

[0717] The propylene polymer (A3) is desired to have MFR, as measured at0.230° C. under a load of 2.16 kg, of 0.01 to 30 g/10 min, preferably0.5 to 5 g/10 min, and Mw/Mn, as measured by GPC, of 4 to 15, preferably4 to 8.

[0718] Further, the propylene polymer (A3) is desired to have anintrinsic viscosity [η] of 1.7 to 5.0 dl/g, preferably 2.2 to 3.5 dl/g,a weight-average molecular weight of 15×10⁴ to 100×10⁴, preferably25×10⁴ to 50×10⁴, a crystallinity, as measured by X-ray diffractometry,of not less than 55%, preferably not less than 60%, and a boilingheptane extraction residue proportion (I.I.) of not less than 90%,preferably not less than 93%.

[0719] The propylene polymer (A3) may contain constituent units derivedfrom monomers other than propylene, which are exemplified for thepropylene polymer (A1), in an amount of not more than 5% by mol.

[0720] Propylene Polymer (A2)

[0721] The propylene polymer (A2) for constituting the third propylenepolymer composition is identical with the propylene polymer (A2) forconstituting the above-mentioned first propylene polymer composition.

[0722] Propylene Polymer Composition

[0723] The third propylene polymer composition comprises the propylenepolymer (A3) and the propylene polymer (A2). In this composition, it isdesired that the propylene polymer (A3) is contained in an amount of 10to 90% by weight, preferably 30 to 70% by weight; and the propylenepolymer (A2) is contained in an amount of 10 to 90% by weight,preferably 30 to 70% by weight. A ratio [(A2)/(A3)] of the MFR of thepropylene polymer (A2) to the MFR of the propylene polymer (A3) is notless than 30, preferably in the range of 40 to 100.

[0724] The third propylene polymer composition is desired to have MFR,as measured at 230° C. under a load of 2.16 kg, of 1 to 100 g/10 min,preferably 5 to 50 g/10 min. In this composition, Mw/Mn of all thepropylene components for constituting the composition is desirably inthe range of 5 to 15.

[0725] The density of the third propylene polymer composition is desiredto be in the range of 0.89 to 0.92 g/cm³, preferably 0.90 to 0.92 g/cm³.

[0726] The heat distortion temperature (HDT) thereof is desired to benot lower than 100° C., preferably in the range of 110 to 150° C.

[0727] The flexural modulus (FM) thereof is desired to be in the rangeof 14,000 to 21,000 kg/cm², preferably 16,000 to 20,000 kg/cm².

[0728] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 2 to 4 kg·cm/cm, preferably 2 to 3 kg·cm/cm.

[0729] The tensile elongation at break (EL) thereof is desired to be inthe range of 100 to 500%, preferably 200 to 400%.

[0730] The third propylene polymer composition may contain, ifnecessary, additives which may be added to the first propylene polymercomposition, with the proviso that the object of the invention is notmarred.

[0731] The third propylene polymer composition can be prepared by knownprocesses. For example, the composition can be prepared in accordancewith the processes (1) to (4) described for the first propylene polymercomposition, using the propylene polymer (A3), the propylene polymer(A2) and if desired other components which may be optionally added.

[0732] The third propylene polymer composition as mentioned above isexcellent in not only heat resistance, rigidity and tensile elongationat break but also moldability.

[0733] Next, the olefin polymerization catalyst used for preparing thepropylene polymer (A3) and the process for preparing the propylenepolymer (A3) are described.

[0734] The propylene polymer (A3) can be prepared bypolymerizing-propylene in the presence of an olefin polymerizationcatalyst [olefin polymerization catalyst (0.2)] comprising:

[0735] (d) a solid titanium catalyst component, and

[0736] (e) an organometallic compound catalyst component.

[0737]FIG. 2 illustrates steps of a process for preparing the olefinpolymerization catalyst which is used for the preparation of thepropylene polymer (A3).

[0738] As the solid titanium catalyst component (d), solid titaniumcatalyst components containing titanium, magnesium and halogen, and, ifdesired, an electron donor (k), can be used.

[0739] The solid titanium catalyst component (d) can be prepared by, forexample, bringing a titanium compound, a magnesium compound and anoptional electron donor (k) into contact with each other.

[0740] The titanium compounds used in the preparation of the solidtitanium catalyst component (d) include, for example, tetravalenttitanium compounds or trivalent titanium compounds.

[0741] The tetravalent titanium compounds include compounds representedby the following formula:

Ti(OR)_(q)X_(4-q)

[0742] wherein R is a hydrocarbon group, X is a halogen atom, and g is anumber satisfying the condition of 0≦g≦4.

[0743] Of these compounds, preferred are titanium tetrahalides, andparticularly preferred is titanium tetrachloride. These titaniumcompounds may be used singly or in combination. Further, they may bediluted in hydrocarbon compounds or halogenated hydrocarbon compounds.

[0744] The trivalent titanium compoun is, for example, titaniumtrichloride.

[0745] The magnesium compound used for preparing the solid titaniumcatalyst component (d) includes a magnesium compound having reductionproperties and a magnesium compound having no reduction properties.

[0746] The magnesium compounds having reduction properties includeorgano-magnesium compounds represented by the following general formula:

X_(n)MgR_(2-n)

[0747] wherein n is a number satisfying the condition of 0≦n<2, R ishydrogen, an alkyl group of 1 to 20 carbon atoms, aryl group orcycloalkyl group (when n is 0, two of R are the same or different), anda hydrocarbon group.

[0748] Concrete examples of the magnesium compound having reductionproperties include dialkylmagnesium compounds, alkylmagnesium halides,alkylmagnesium alkoxides and butylmagnsium hydride.

[0749] Concrete examples of the magnesium compound having no reductionproperties include magnesium halide such as magnesium chloride,magnesium bromide, magnesium iodide and magnesium fluoride;alkoxymagnesium halide; aryloxymagnesium halide; alkoxymagnesium;aryloxymagnesium; and manesium carboxylate. Further, magnesium metal orhydrogenated magnesium may also be used.

[0750] These magnesium compounds having no reduction properties may bethose derived from the above-mentioned magnesium compounds havingreduction properties or those derived during the catalyst componentpreparation stage. In order to derive the magnesium compound having noreduction properties from the magnesium compound having reductionproperties, the magnesium compound having reduction properties isbrought into contact with a polysiloxane compound, a halogen-containingsilane compound, a halogen-containing aluminum compound, an ester, analcohol, halogen-containing compound or a compound having an OH-group oran active carbon-oxygen bond.

[0751] The magnesium compounds may be used singly or in combination oftwo or more kinds, an in any of liquid state or solid state. When themagnesium compound is solid, the compound can be brought into liquidstate by using the electron donors as same as those described in later,such as alcohols, carboxylic acids, aldehydes, amins or metal acidesters.

[0752] In the preparation of the solid titanium catalyst component (d),an electron donor (k) is preferably used. Examples of the electron donor(k) include:

[0753] oxygen-containing electron donors such as alcohols, phenols,ketones, aldehydes, carboxylic acids, organic acid halides, esters oforganic acids or inorganic acids, ethers, diethers, acid amides, acidanhydrides and alkoxysilanes, and

[0754] nitrogen-containing donors such as an ammonia, amines, nitrites,pyridines and isocyanates.

[0755] The solid titanium catalyst component (d) is prepared by bringingthe aforementioned titanium compound, magnesium compound and theoptional electron donor (k) into contact with each other.

[0756] Though the processes for preparing the solid titanium catalystcomponent (d) are no way limited, examples of such processes by usingthe tetravalent titanium compound are briefly described below.

[0757] (1) A process comprising bringing a solution consisting of amagnesium compound, an electron donor (k) and a hydrocarbon solvent intocontact with an organometallic compound, after or simultaneously withprecipitating a solid by bringing the solution into contact with atitanium compound.

[0758] (2) A process comprising bringing a complex composed of amagnesium compound and an electron donor (k) into contact with anorganometallic compound, and then bringing the reaction product intocontact with a titanium compound.

[0759] (3) A process comprising bringing a product obtained by thecontact of an inorganic carrier and an organic magnesium compound intocontact with a titanium compound. In this case, the above product may bebeforehand brought into contact with a halogen-containing compound, anelectron donor (k) and/or an organometallic compound.

[0760] (4) A process comprising obtaining an inorganic or organiccarrier on which a magnesium compound is supported from a mixture of aninorganic or organic carrier and a solution containing a magnesiumcompound and an electron donor (k) (and further a hydrocarbon solvent insome cases), and then bringing the obtained carrier into contact with atitanium compound.

[0761] (5) A process comprising bringing a solution containing amagnesium compound, a titanium compound and an electron donor (k) (andfurther a hydrocarbon solvent in some cases) into contact with aninorganic or organic carrier to obtain a solid titanium catalystcomponent on which magnesium and titanium are supported.

[0762] (6) A process comprising bringing a liquid organic magnesiumcompound into contact with a halogen-containing titanium compound.

[0763] (7) A process comprising bringing a liquid organic magnesiumcompound into contact with a halogen-containing compound, and thenbringing the product thus obtained into contact with atitanium-compound.

[0764] (8) A process comprising bringing an alkoxy group-containingmagnesium compound into contact with a halogen-containing titaniumcompound.

[0765] (9) A process comprising bringing a complex composed of an alkoxygroup-containing magnesium compound and an electron donor (k) intocontact with a titanium compound.

[0766] (10) A process comprising bringing a complex composed of analkoxy group-containing magnesium compound and an electron donor (k)into contact with an organometallic compound, and then bringing theproduct thus obtained into contact with a titanium compound.

[0767] (11) A process comprising bringing a magnesium compound, anelectron donor (k) and a titanium compound into contact with each otherin an optional order. In this reaction, each components may bepretreated with an electron donor (k) and/or a reaction assistant suchas an organometallic compound or a halogen-containing silicon compound.In this case, an electron donor is preferably used at least one time

[0768] (12) A process comprising bringing a liquid magnesium compoundnot having reducing ability into contact with a liquid titaniumcompound, if necessary in the presence of an electron donor (k), toprecipitate a solid magnesium/titanium complex compound.

[0769] (13) A process comprising further bringing the reaction productobtained in the above process (12) into contact with an titaniumcompound.

[0770] (14) A process comprising further bringing the reaction productobtained in the above process (11) or (12) into contact with an electrondonor (k) and a titanium compound.

[0771] (15) A process comprising pulverizing a magnesium compound and atitanium compound (and if necessary an electron donor (k)) to obtain asolid product, and treating the solid product with either halogen, ahalogen compound or aromatic hydrocarbon. This process may include astep of pulverizing only a magnesium compound, a step of pulverizing acomplex compound composed of a magnesium compound and an electron donor(k), or a step of pulverizing a magnesium compound and a titaniumcompound. Further, after the pulverization, the solid product may besubjected to a pretreatment with a reaction assistant and then subjectedto a treatment with halogen or the like. Examples of the reactionassistants include an organometallic compound and a halogen-containingsilicon compound.

[0772] (16) A process comprising pulverizing a magnesium compound, andthen bringing the pulverized magnesium compound into contact with atitanium compound. In this case, an electron donor (k) or a reactionassistant may be used in the pulverization stage and/or the contactingreaction stage.

[0773] (17) A process comprising treating the compound obtained in anyof the above processes (11) to (16) with halogen, a halogen compound oraromatic hydrocarbon.

[0774] (18) A process comprising bringing the reaction product obtainedby the contact of a metal oxide, an organic magnesium compound and ahalogen-containing compound into contact with a titanium compound and ifnecessary an electron donor (k).

[0775] (19) A process comprising bringing a magnesium compound such as amagnesium salt of organic acid, alkoxymagnesium or aryloxymagnesium intocontact with a titanium compound and/or halogen-containing hydrocarbonand if necessary an electron donor (k).

[0776] (20) A process comprising bringing a hydrocarbon solutioncontaining at least a magnesium compound and alkoxytitanium into contactwith a titanium compound and/or an electron donor (k). In this case, ahalogen-containing compound such as a halogen-containing siliconcompound may be further brought into contact therewith, if necessary.

[0777] (21) A process comprising bringing a liquid magnesium compoundnot having reducing ability into contact with an organometallic compoundso as to precipitate a solid magnesium/metal (aluminum) complexcompound, and then bringing the resulting compound into contact with anelectron donor (k) and a titanium compound.

[0778] The preparation of the solid titanium catalyst component (d) isconducted at a temperature of usually −70 to 200° C., preferably −50 to150° C.

[0779] The solid titanium catalyst component (d) thus obtained containstitanium, magnesium, halogen and an optional electron donor.

[0780] In the solid titanium catalyst component (d), a ratio ofhalogen/titanium (atomic ratio) is about 2 to 200, preferably about 4 to90, a ratio of magnesium/titanium (atomic ratio) is 1 to 100, preferably2 to 50.

[0781] Further, the electron donor (k) is containined in a ratio ofelectron donor (k)/titanium (molar ratio) being about 0.01 to 100,preferably about 0.05 to 50.

[0782] Regarding the processes for preparation of the solid titaniumcatalyst component (d), details thereof are described in the followingpublications;

[0783] JP-B-46-34092/1971, JP-B-53-46799/1978, JP-B-60-3323/1985,JP-B-63-54289/1988, JP-A-1-261404/1989, JP-A-1-261407/1989,JP-B-47-41676/1972, JP-B-47-46269/1972, JP-B-19794/1973,JP-A-60-262803/1985, JP-A-59-147004/1984, JP-A-59-149911/1984,JP-A-1-201308/1989, JP-A-61-151211/1986, JP-A-53-58495/1978,JP-A-53-87990/1978, JP-A-59-206413/1984, JP-A-58-206613/1983,JP-A-58-125706/1983, Jp-A-63-68606/1988, JP-A-63-69806/1988,JP-A-60-81210/1985, JP-A-61-40306/1986, JP-A-51-281189/1976,JP-A-50-126590/1975, JP-A-51-92885/1976, JP-B-57-45244/1982,JP-B-57-26613/1982, JP-B-61-5483/1986, JP-A-56-811/1981,JP-B-60-37804/1985, JP-B-59-50246/1984, JP-A-58-83006/1983,JP-A-48-16986/1973, JP-A-49-65999/1974, JP-A-49-86482/1974,JP-B-56-39767/1981, JP-B-56-32322/1981, JP-A-55-29591/1980,JP-A-53-146292/1978, JP-A-57-63310/1982, JP-A-57-63311/1982,JP-A-57-63312/1982, JP-A-62-273206/1987, JP-A-63-69804/1988,JP-A-61-21109/1986, JP-A-63-264607/1988, JP-A-60-23404/1985,JP-A-60-44507/1985, JP-A-60-158204/1985, JP-A-61-55104/1986,JP-A-2-28201/1990, JP-A-58-196210/1983, JP-A-64-54005/1989,JP-A-59-149905/1984, JP-A-61-145206/1986, JP-A-63-302/1988,JP-A-63-225605/1988, JP-A-64-69610, JP-A-1-168707/1989,JP-A-62-104810/1987, JP-A-62-104811/1987, JP-A-62-104812/1987 andJP-A-62-104813/1987.

[0784] In the present invention, conventional titanium trichloride typecatalyst component may also be used as the solid titanium catalystcomponent (d).

[0785] The above mentioned titanium trichloride is exemplified as thetitanium trichloride type catalyst component. The titanium trichlorideis used together with the aforementioned electron donor (k) and/or thetetravalent titanium compound, or after the contact with them.

[0786] Regarding the processes for preparation of the titaniumtrichloride type catalyst component, details thereof are described inthe following publications;

[0787] JP-A-63-17274/1988, JP-A-64-38409/1989, JP-A-56-34711/1981,JP-A-61-287904/1986, JP-A-63-75007/1988, JP-A-63-83106/1988,JP-A-59-13630/1984, JP-A-63-108008/1988, JP-A-63-27508/1988,JP-A-57-70110/1982, JP-A-58-219207/1983, JP-A-1-144405/1989 andJP-A-1-292011/1989.

[0788] Embodiment of the titanium trichloride type catalyst componentincludes titanium trichloride. As the titanium trichloride, there can bepreferably used a titanium trichloride which is obtained by, forexample, reducing the tetravalent titanium by contacting with hydrogen,metal such as magnesium metal, aluminum metal or titanium metal, or anorganic metal compound such as organomagnesium compound, organoaluminumcompound or organozinc compound. The titanium trichloride is usedtogether with the aforementioned electron donor (k) and/or thetetravalent titanium compound, or after the contact with them.

[0789] Examples of the organometallic compound catalyst component (e)which forms the olefin polymerization catalyst (2) used in thepolymerization of the propylene polymer (A3) include (e-1) anorganoaluminum compound, (e-2) a complex alkyl compound of aluminum withGroup I metal of the periodic table and (e-3) a organometallic compoundof Group II metal of the periodic table.

[0790] Examples of the organoaluminum compound (e-1) are the same asthose described as the organoaluminum (j).

[0791] Examples of the complex alkyl compound of aluminum with Group Imetals of the periodic table (e-2) are represented by the followinggeneral formula;

M¹AlR^(j) ₄

[0792] wherein M¹ is Li, Na or K and R^(j) is a hydrocarbon group of 1to 15 carbon atoms.

[0793] Examples of the organometallic compound of Group II metal of theperiodic table (e-3) are represented by the following general formula;

R^(k)R¹M²

[0794] wherein R^(k) and R¹ are hydrocarbon group of 1 to 15 carbonatoms or halogen, and they being the same or different with a provisothat excluding the case where the each of them is halogen, and M² is Mg,Zn or Cd.

[0795] These compounds may be used in combination of 2 or more kinds.

[0796] In the preparation of the propylene polymer (A3), the aforesaidorganoaluminum oxy-compound (b) can be also employed.

[0797] The propylene polymer (A3) can be prepared by polymerizingpropylene in the presence of the olefin polymerization catalyst (2)formed from the solid titanium catalyst component (d) and theorganometallic compound catalyst component (e).

[0798] The olefin polymerization catalyst (2) may be a prepolymerizedcatalyst obtained by prepolymerizing the catalyst comprising the solidtitanium catalyst component (d) and the organometallic compound catalystcomponent (e) with an olefin.

[0799] Examples of the olefins used for the prepolymerization includeα-olefins of 2 to 20 carbon atoms. Of these, propylene is preferred.

[0800] In the prepolymerization, the same electron donor as theaforementioned electron donor (k) or the following electron donor (1)may be used if necessary, in addition to the catalyst component (d) andthe catalyst component (e).

[0801] The electron donor (1) is, for example, an organosilicon compoundrepresented by the following formula:

R_(n)Si(OR′)_(4-n)

[0802] wherein R and R′ are each a hydrocarbon group, and 0<n<4.

[0803] The organosilicon compound represented by the above formulaincludes the following compounds.

[0804] These organosilicon compounds may be used in combination of twoof more kinds. Also employable as the electron donor (1) are:nitrogen-containing electron donors, such as 2,6-substitutedpiperidines, 2,5-substituted piperidines, substituted methylenediaminesand substituted imidazolidines;

[0805] phosphorus-containing electron donors, such as phosphites; and

[0806] oxygen-containing electron donors, such as 2,6-substitutedtetrahydropyrans and 2,5-substituted tetrahydropyrans.

[0807] In the prepolymerization, the olefin is desirably polymerized inan amount of usually 0.01 to 2,000 g, preferably 0.03 to 1,000 g,particularly preferably 0.05 to 200 g, per 1 g of the solid titaniumcatalyst component (d).

[0808] The prepolymerized catalyst prepared as above is usually obtainedin the form of a suspension. In the subsequent polymerization step, suchprepolymerized catalyst may be used in the form of the suspension.Otherwise, the prepolymerized catalyst produced may be separated fromthe suspension before use.

[0809] When the prepolymerized catalyst is used for the polymerizationto prepare the propylene polymer (A3), the organometallic compoundcatalyst component (e) is preferably used in combination with theprepolymerized catalyst.

[0810] The propylene polymer (A3) can be prepared by polymerizingpropylene in the presence of the olefin polymerization catalyst (2). Inthe polymerization of propylene, ethylene and monomers which areexemplified for the propylene polymer (A1) and the propylene polymer(A2), such as α-olefins of 4 to 20 carbon atoms, may be used in amountsof not more than 0.1 mol per 1 mol of propylene.

[0811] The propylene polymer. (A3) may be prepared by either a liquidphase polymerization process such as a solution polymerization processand a suspension polymerization process, or a gas phase polymerizationprocess.

[0812] When the polymerization is conducted in the reaction form ofsuspension polymerization, polyene compounds and olefins which areliquid at reaction temperatures and/or the same inert solvents as usedfor the aforementioned prepolymerization can be used as the reactionsolvent.

[0813] The olefin polymerization catalyst (2) used for thepolymerization is generally used in the following amount, though theamount varies depending upon the kind.

[0814] The solid titanium catalyst component (d) (including theprepolymerized catalyst) is used in an amount of usually about 0.001 to100 mmol, preferably about 0.005 to 20 mmol, in terms of the titaniumatom in the solid titanium catalyst component (d) or the prepolymerizedcatalyst, based on 1 liter of the polymerization volume.

[0815] The organometallic compound catalyst component (e) is used insuch an amount that the amount of the metal atom in said catalystcomponent (e) is in the range of usually about 1 to 2,000 mol,preferably about 5 to 500 mol, based on 1 mol of the titanium atom inthe solid titanium catalyst component (d) or the prepolymerizedcatalyst.

[0816] The electron donors (k) and (1) may be also employed in additionto the catalyst component (d) and the catalyst component (e). When theelectron donor is used, the amount of the electron donor is in the rangeof usually about 0.001 to 10 mol, preferably 0.01 to 5 mol, based on 1mol of the metal atom in the organometallic compound catalyst component(e)

[0817] The olefin polymerization catalyst (2) may contain othercomponents than the above-mentioned components, which are useful for theolefin polymerization.

[0818] The molecular weight of the resulting polymer may be regulated ifhydrogen is used in the polymerization, and thereby a polymer having ahigh melt flow rate can be obtained.

[0819] The polymerization is generally carried out under the followingconditions. The polymerization temperature is in the range of about −40to 300° C., preferably about −20 to 150° C., and the polymerizationpressure is in the range of atmospheric pressure to 100 kg/cm²,preferably about 2 to 50 kg/cm².

[0820] The polymerization can be carried out either batchwise,semi-continuously or continuously. Further, the polymerization can beconducted in two or more steps, and in this case, the reactionconditions may be the same as or different from each other.

The Fourth Propylene Polymer Composition

[0821] The fourth propylene polymer composition comprises:

[0822] (A3) a propylene polymer which is prepared by the use of anolefin polymerization catalyst comprising the solid titanium catalystcomponent (d) and the organometallic compound catalyst component (e),and which has MFR, as measured at 230° C. under a load of 2.16 kg, of0.01 to 30 g/10 min, and a molecular weight distribution (Mw/Mn), asmeasured by GPC, of 4 to 15;

[0823] (A2) a propylene polymer which is characterized in that:

[0824] the propylene polymer is prepared by the use of an olefinpolymerization catalyst comprising:

[0825] (i) (a) a transition metal compound and

[0826] (ii) at least one compound selected from the group consisting of

[0827] (b) an organoaluminum oxy-compound, and

[0828] (c) a compound which reacts with the transition metal compound(a) to form an ion pair,

[0829] the propylene polymer has MFR, as measured at 230° C. under aload of 2.16 kg, of 30 to 1,000 g/10 min, and

[0830] the propylene polymer has a molecular weight distribution(Mw/Mn), as measured by GPC, of 2 to 4; and.

[0831] (B) a soft polymer.

[0832] Propylene Polymer (A3)

[0833] The propylene polymer (A3) for constituting the fourth propylenepolymer composition is identical with the propylene polymer (A3) forconstituting the above-mentioned third propylene polymer composition.

[0834] Propylene Polymer (A2)

[0835] The propylene polymer (A2) for constituting the fourth propylenepolymer composition is identical with the propylene polymer (A2) forconstituting the above-mentioned first propylene polymer composition.

[0836] Soft Polymer (B)

[0837] The soft polymer (B) for constituting the fourth propylenepolymer composition is identical with the soft polymer (B) forconstituting the above-mentioned second propylene polymer composition.

[0838] Propylene Polymer Composition

[0839] The fourth propylene polymer composition comprises the 0.5propylene polymer (A3), the propylene polymer (A2) and the soft polymer(B). In this composition, it is desired that the propylene polymer (A3)is contained in an amount of 10 to 90 parts by weight, preferably 30 to70 parts by weight; the propylene polymer (A2) is contained in an amountof 10 to 90 parts by weight, preferably 30 to 70 parts by weight; andthe soft polymer (B) is contained in an amount of 3 to 30 parts byweight, preferably 10 to 25 parts by weight. A ratio [(A2)/(A3)] of theMFR of the propylene polymer (A2) to the MFR of the propylene polymer(A3) is not less than 30, preferably in the range of 40 to 100.

[0840] The fourth propylene polymer composition is desired to have MFR,as measured at 230° C. under a load of 2.16 kg, of 1 to 100 g/10 minpreferably 5 to 50 g/10 min. In this composition, Mw/Mn of all thepropylene components for constituting the composition is desirably inthe range of 5 to 15.

[0841] The density of the fourth propylene polymer composition isdesired to be in the range of 0.88 to 0.92 g/cm³; preferably 0.89 to0.92 g/cm³.

[0842] The heat distortion temperature (HDT) thereof is desired to benot lower than 85° C., preferably in the range of 95 to 140° C.

[0843] The flexural modulus (FM) thereof is desired to be in the rangeof 8,500 to 18,000 kg/cm², preferably 9,000 to 15,000 kg/cm².

[0844] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 10 to 50 kg·cm/cm, preferably 10 to 40 kg·cm/cm.

[0845] The tensile elongation at break (EL) thereof is desired to be inthe range of 200 to 1,000%, preferably 300 to 500%.

[0846] The fourth propylene polymer composition may contain theaforesaid additives, if necessary, with the proviso that the object ofthe invention is not marred.

[0847] The fourth propylene polymer composition can be prepared by knownprocesses. For example, the composition can be prepared in accordancewith the processes (1) to (4) described for the first propylene polymercomposition, using the propylene polymer (A3), the propylene polymer(A2), the soft polymer (B) and if desired other components which may beoptionally added.

[0848] The Fifth Propylene Polymer Composition

[0849] The fifth propylene polymer composition according to theinvention comprises:

[0850] (A4) a propylene polymer which-is prepared by the use of acatalyst comprising (d) the solid titanium catalyst component and (e)the organometallic compound catalyst component, and which has MFR, asmeasured at 230° C. under a load of 2.16 kg, of 0.01 to 50 g/10 min, amolecular weight distribution (Mw/Mn), as measured by GPC, of 4 to 15and a crystallinity, as measured by X-ray diffractometry, of not lessthan 50%; and

[0851] (C) an ethylene/olefin random copolymer which is characterized inthat:

[0852] the copolymer is prepared by the use Qf a catalyst comprising:

[0853] (i) (f) a transition metal compound containing a ligand having acyclopentadienyl skeleton,

[0854] (ii) at least one compound selected from the groups consisting of

[0855] (b) an organoaluminum oxy-compound, and

[0856] (g) a compound which reacts with the transition metal compound(f) to form an ion pair,

[0857] the copolymer contains constituent units derived from ethylene inan amount of 20 to 80% by mol, and

[0858] the copolymer has an intrinsic viscosity [η], as measured indecalin at 135° C., of 1.5 to 5 dl/g.

[0859] Propylene Polymer (A4)

[0860] The propylene polymer (A4) is a propylene homopolymer or apropylene copolymer, and desirably has MFR, as measured at 230° C. undera load of 2.16 kg, of 0.01 to 50 g/10 min, preferably 1 to 30 g/10 min.The molecular weight distribution (Mw/Mn) of this propylene polymer, asmeasured by GPC, is desired to be in the range of 4 to 15, preferably 4to 8. Further, this propylene polymer is desired to have acrystallinity, as measured by X-ray diffractometry, of not less than50%, more preferably not less than 60%, and to be highly crystalline.

[0861] The propylene polymer (A4) is desired to have an intrinsicviscosity [η], as measured in decalin at 135° C., of 1.3 to 5.0 dl/g,preferably 1.4 to 3.0 dl/g, a weight-average molecular weight of 12×10⁴to 100×10⁴, preferably 13×10⁴ to 40×10⁴, and a boiling heptaneextraction residue proportion (I.I.) of not less than 90%, preferablynot less than 93%.

[0862] The propylene polymer (A4) may contain constituent units derivedethylene and α-olefins of 4 to 20 carbon atoms in an amount of not morethan 5% by mol.

[0863] Examples of the α-olefins of 4 to 20 carbon atoms include1-butene, 1-pentene, 1-hexene, 3-methyl-1-butene, 3-methyl-1-pentene,3-ethyl-1-pentene, 4-methyl-1-pentene, 4-methyl-1-hexene,4,4-dimethyl-1-hexene, 4,4-dimethyl-1-pentene, 4-ethyl-1-hexene,3-ethyl-1-hexene, 1-octene, 1-decene, 1-dodecene, 1-tetradecene,1-hexadecene, 1-octadecene and 1-eicosene.

[0864] Ethylene/Olefin Random Copolymer (C)

[0865] The ethylene/olefin random copolymer (C) contains constituentunits derived from ethylene in an amount of 20 to 80% by mol, preferably30 to 60% by mol, and contains constituent units derived from at leastone monomer (olefin) selected from α-olefins of 3 to 20 carbon atoms andpolyenes of 5 to 20 carbon atoms in an amount of 80 to 20% by mol,preferably 70 to 40% by mol.

[0866] Examples of the α-olefins of 3 to 20 carbon atoms includepropylene, 1-butene, 1-pentene, 1-hexene, 4-methyl-1-pentene, 1-octene,1-decene, 1-dodecene, 1-tetradecene, 1-hexadecene and 1-octadecene. Ofthese, propylene is preferred. These α-olefins may be used singly or incombination of two or more.

[0867] The polyene of 5 to 20 carbon atoms is, for example, a conjugatedor non-conjugated polyene having two or more olefinic double bonds.

[0868] Examples of such polyenes include:

[0869] chain polyene compounds, such as 1,3-pentadiene, 1,4-pentadiene,1,3-hexadiene, 1,4-hexadiene, 1,5-hexadiene, 4-methyl-1,4-hexadiene,5-methyl-1,4-hexadiene, 6-methyl-1,6-octadiene, 7-methyl-1,6-octadiene,6-ethyl-1,6-octadiene, 6-propyl-1,6-octadiene, 6-butyl-1,6-octadiene,6-methyl-1,6-nonadiene, 7-methyl-1,6-nonadiene, 6-ethyl-1,6-nonadiene,7-ethyl-1,6-nonadiene, 6-methyl-1,6-decadiene, 7-methyl-1,6-decadiene,6-methyl-1,6-undecadiene, 1,7-octadiene, 1,9-decadiene,2,4,6-octatriene, 1,3,7-octatriene, 1,5,9-decatriene and divinylbenzene;and

[0870] cyclic polyene compounds, such as 1,3-cyclopentadiene,1,3-cyclohexadiene, 5-ethyl-1,3-cyclohexadiene, 1,3-cycloheptadiene,dicyclopentadiene, dicyclohexadiene, 5-ethylidene-2-norbornene,5-vinyl-2-norbornene, 5-isopropylidene-2-norbornene, methylhydroindene,2,3-diisopropylidene-5-norbornene,2-ethylidene-3-isopropylidene-5-norbornene,2-ethylidene-3-isopropylidene-5-norbornene and2-propenyl-2,5-norbornadiene.

[0871] The ethylene/olefin random copolymer (C) has an intrinsicviscosity [η], as measured in decalin at 135° C., of 1.5 to 5 dl/g,preferably 2.0 to 4.0 dl/g.

[0872] The ethylene/olefin random copolymer (C) desirably has amolecular weight distribution (Mw/Mn), as measured by GPC, of notmore-than 3.0, preferably 2.0 to 2.5.

[0873] Further, the ethylene/olefin random copolymer (C) is desired tohave a glass transition temperature (Tg) of not higher than −40° C.,preferably not higher than −50° C.

[0874] The ethylene/olefin random copolymer (C) is desired to be lowlycrystalline or amorphous, and to have a crystallinity, as measured byX-ray diffractometry, of not more than 30%, preferably 0 to 10%.

[0875] Propylene Polymer Composition

[0876] The fifth propylene polymer composition comprises the propylenepolymer (A4) and the ethylene/olefin random copolymer (C). In thiscomposition, it is desired that the propylene polymer (A4) is containedin an amount of 50 to 97% by weight, preferably 70 to 90% by weight; andthe ethylene/olefin random copolymer (C) is contained in an amount of 3to 50% by weight, preferably 10 to 30% by weight.

[0877] The fifth propylene polymer composition is desired to have MFR,as measured at 230° C. under a load of 2.16 kg, of 0.01 to 100 g/10 min,preferably 1 to 50 g/10 min. In this composition, Mw/Mn of all thepropylene components for constituting the composition is desirably inthe range of 4 to 15.

[0878] The density of the fifth propylene polymer composition is desiredto be in the range of 0.88 to 0.92 g/cm³, preferably 0.89 to 0.92 g/cm³.

[0879] The flexural-modulus (FM) thereof is desired to be in the rangeof 8,000 to 17,000 kg/cm², preferably 9,000 to 15,000 kg/cm².

[0880] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 10 to 50 kg·cm/cm, preferably 10 to 40 kg·cm/cm, and at−30° C. in the range of 5 to 15 kg·cm/cm, preferably-7 to 15 kg·cm/cm.

[0881] The tensile elongation at break (EL) thereof is desired to be inthe range of 200 to 500%, preferably 250 to 450%.

[0882] The heat distortion temperature (HDT) thereof is desired to benot lower than 80° C., preferably in the range of 90 to 110° C.

[0883] The fifth propylene polymer composition may contain, ifnecessary, additives which may be added to the first propylene polymercomposition, with the proviso-that the object of the invention is notmarred.

[0884] The fifth propylene polymer composition can be prepared by knownprocesses. For example, the composition can be prepared in accordancewith the processes (1) to (4) described for the first propylene polymercomposition, using the propylene polymer (A4) and the ethylene/olefinrandom copolymer (C).

[0885] Such fifth propylene polymer composition is excellent in not onlyheat resistance and rigidity but also mechanical strength such asflexural strength and impact resistance.

[0886] The fifth propylene polymer composition is excellent especiallyin the low-temperature impact resistance as compared with a propylenepolymer composition comprising a propylene polymer and anethylene/olefin random copolymer prepared by the use of a conventionaltitanium catalyst.

[0887] The fifth propylene polymer composition can be favorably used forstructural materials such as those of automobiles and electricalappliances.

[0888] Next, the catalyst used for the preparation of the propylenepolymer (A4), the process for preparing said catalyst, the catalyst usedfor the preparation of the ethylene/olefin random copolymer and theprocess for preparing said catalyst are described.

[0889] The propylene polymer (4) is obtained by polymerizing propylenein the presence of an olefin polymerization catalyst comprising thesolid titanium catalyst component (d) and the organometallic compoundcatalyst component (e), said catalyst being the same as the olefinpolymerization catalyst (2) which is used for the preparation of thepropylene polymer (A3).

[0890] In the polymerization of propylene, other monomers thanpropylene, such as ethylene and the aforesaid α-olefins of 4 to 20carbon atoms, may be used in the amounts of not more than 0.1 mol basedon 1 mol of propylene.

[0891] The propylene polymer (A4) can be prepared by either a liquidphase polymerization process such as a solution polymerization processand a suspension polymerization process, or a gas phase polymerizationprocess.

[0892] When the polymerization is conducted in the reaction form of thesuspension polymerization, polyene compounds and olefins which areliquid at reaction temperatures and/or the same inert solvents as usedfor the preparation of the olefin polymerization catalyst (1) can beused as the reaction solvent.

[0893] The olefin polymerization catalyst used for the polymerization isgenerally used in the following amount, though the amount variesdepending upon the kind.

[0894] The solid titanium catalyst component-(d) (including-theprepolymerized catalyst) is used in an amount of usually about 0.001 to100 mmol, preferably about 0.005 to 20 mmol, in terms of the titaniumatom in the solid titanium catalyst component (d) or the prepolymerizedcatalyst, based on 1 liter of the polymerization volume.

[0895] The organometallic compound catalyst component (e) is used insuch an amount that the amount of the metal atom in said catalystcomponent (e) is in the range of usually about 1 to 2,000 mol,preferably about 5 to 500 mol, based on 1 mol of the titanium atom inthe solid titanium catalyst component (d) or the prepolymerizedcatalyst.

[0896] The same electron donors as the aforesaid electron donors (k) and(1) may be also employed in addition to the catalyst component (d) andthe catalyst component (e).

[0897] When the electron donor is used, the amount of the electron donoris in the range of usually about 0.001 to 10 mol, preferably 0.01 to 5mol, based on 1 mol of the metal atom in the organometallic compoundcatalyst component (e).

[0898] The olefin polymerization catalyst used for preparing thepropylene polymer (A4) may contain other components than theabove-mentioned components, which are useful for the olefinpolymerization.

[0899] The molecular weight of the resulting polymer can be regulated ifhydrogen is used in the polymerization, whereby a polymer having a highmelt flow rate can be obtained.

[0900] The polymerization is generally carried out under the followingconditions. The polymerization temperature is in the range of about −40to 300-° C., preferably about −20 to 150° C., and the polymerizationpressure is in the range of atmospheric pressure to 100 kg/cm²,preferably about 2 to 50 kg/cm².

[0901] The polymerization can be carried out either batchwise,semi-continuously or continuously. Further, the polymerization can beconducted in two or more steps, and in this case, the reactionconditions may be the same as or different from each other.

[0902] The ethylene/olefin random copolymer (C) is obtained bycopolymerizing ethylene and at least one monomer (olefin) selected froman α-olefin of 3 to 20 carbon atoms and a polyene of 5 to 20 carbonatoms in the presence of an olefin polymerization catalyst [olefinpolymerization catalyst (3)] comprising:

[0903] (i) (f) a transition metal compound containing a ligand having acyclopentadienyl skeleton, and

[0904] (ii) at least one compound selected from the group consisting of

[0905] (b) an organoaluminum oxy-compound, and

[0906] (g) a compound which reacts with the transition metal compound(f) to form an ion pair.

[0907]FIG. 3 illustrates steps of a process for preparing the olefinpolymerization catalyst which is used for the preparation of theethylene/olefin random copolymer (C).

[0908] Examples of the transition metal compound (f) having acyclopentadienyl skeleton include the transition metal compound (h)represented by the aforementioned formula (I) and the compoundrepresented by the following formula (Ic).

ML_(x)  (Ic)

[0909] wherein M is a transition metal atom selected from the groupconsisting of zirconium, titanium, hafnium, vanadium, niobium, tantalumand chromium, L is a ligand coordinating to the transition metal, atleast one of L is a ligand having a cyclopentadienyl skeleton, and Lother than the ligand having a cyclopentadienyl skeleton is ahydrocarbon group of 1-12 carbon atoms, an alkoxy group, an aryloxygroup, a trialkylsilyl group SO₃R group (provided that R is ahydrocarbon group of 1-8 carbon atoms which may have such a substituentas halogen), halogen atom or hydrogen atom, and x is a valence of thetransition metal atom.

[0910] The ligands having a cyclopentadienyl skeleton are, for example,cyclopentadienyl group, alkyl-substituted cyclopentadienyl groups suchas methylcyclopentadienyl, dimethylcyclopentadienyl,trimethylcyclopentadienyl, tetramethylcyclopentadienyl,pentamethylcyclopentadienyl, ethylcyclopentadienyl,methylethylcyclopentadienyl, propylcyclopentadienyl,methylpropylcyclopentadienyl, butylcyclopentadienyl,methylbutylcyclopentadienyl and hexylpentadienyl, or indenyl group,4,5,6,7-tetrahydroindenyl group and fluorenyl group. These groups asexemplified above may be substituted with a halogen atom ortrialkylsilyl group.

[0911] Of the ligands coordinating with the transition metal atom,particularly preferred is an alkyl-substituted cyclopentadienyl group.

[0912] When the compound represented by the formula (Ic) contains 2 ormore ligands each having a cyclopentadienyl skeleton, the two ligandsout of those having a cyclopentadienyl skeleton may be linked togetherthrough an alkylene group such as ethylene or propylene, a substitutedalkylene group such as isopropylidene or diphenylmethylene, a silylenegroup or a substituted silylene group such as dimethylsilylene,diphenylsilylene or methylphenylsilylene.

[0913] The ligands L other than those having a cyclopentadienyl skeletonmay include those mentioned below.

[0914] The hydrocarbon group of 1-12 carbon atoms includes such group asalkyl, cycloalkyl, aryl or aralkyl, and more particularly, the alkylgroup includes methyl, ethyl, propyl, isopropyl or butyl;

[0915] the cycloalkyl group includes cyclopentlyl or cyclohexyl;

[0916] the aryl group includes phenyl or tolyl; and

[0917] the aralkyl group includes benzyl or neophyl

[0918] Further, the alkoxy group includes methoxy, ethoxy or butoxy;

[0919] aryloxy group includes phenoxy;

[0920] the halogen includes fluorine, chlorine, bromine or iodine; and

[0921] the ligand represented by SO₃R includes p-toluenesulfonate,methanesulfonate or trifluoromethanesulfonate.

[0922] When the valence of the transition metal atom is, for example, 4,the transition metal compound is represented by the following formula(Id) in more detail.

[0923] R²kR³¹R⁴mR⁵ nM  (Id)

[0924] wherein M represents the aforementioned transition metal atom, R²represents a group (ligand) having a cyclopentadienyl skeleton, R³, R⁴and R⁵ each represent a group having a cyclopentadienyl skeleton, alkylgroup, cycloalkyl group, aryl group, aralkyl group, alkoxyl group,aryloxy group, trialkylsilyl group, SO₃R group, halogen atom or hydrogenatom, k is an integer of 1 or more, and k+l+m+n=4.

[0925] In the present invention, there is used preferably a metallocenecompound having the above-mentioned formula (Id) in which at least twoof R², R³, R⁴ and R⁵ are the groups (ligands) having a cyclopentadienylskeleton, for example, R² and R³ are the groups (ligands) having acyclopentadienyl. In this case, the groups having a cyclopentadienylskeleton mentioned above may be linked together through an alkylenegroup such as ethylene or propylene, a substituted alkylene group suchas isopropylene or diphenylmethylene, a silylene group or a substitutedsilylene group such as dimethylsilylene, diphenylsilylene ormethylphenylsilylene. Further, R⁴ and R⁵ are each a group having acyclopentadienyl skeleton, alkyl group, cycloalkyl group, aryl group,arlakyl group, alkoxyl group, aryloxy group, trialkylsilyl group, SO₃Rgroup, halogen atom or hydrogen atom.

[0926] Exemplified below are the transition metal compounds wherein M iszirconium.

[0927] Bis(indenyl)zirconium dichloride,

[0928] Bis(indenyl)zirconium dibromide,

[0929] Bis(indenyul)zirconium bis(p-toluenesulfonate),

[0930] Bis(4,5,6,7-tetrahydroindenyl)zirconium dichloride,

[0931] Bis(fluorenyl)zirconium dichloride,

[0932] Ethylenebis(indenyl)zirconium dichloride,

[0933] Ethylenebis(indenyl)zirconium dibromide,

[0934] Ethylenebis(indenyl)dimethylzirconium,

[0935] Ethylenebis(indenyl)diphenylzirconium,

[0936] Ethylenebis(indenyl)methylzirconium monochloride,

[0937] Ethylenebis(indenyl)zirconium bis(methanesulfonate),

[0938] Ethylenebis(indenyl)zirconium bis(p-toluenesulfonate),

[0939] Ethylenebis(indenyl)zirconium bis(trifluoromethanesulfonate),

[0940] Ethylenebis(4,5,6,7-tetrahydroindenyl)zirconium dichloride,

[0941] Isopropylidene (cyclopentadienyl-fluorenyl) zirconium dichloride,

[0942] Isopropylidene(cyclopentadienyl-methylcyclopentadienyl)zirconiumdichloride,

[0943] Dimethylsilylenebis(cyclopentadienyl)zirconium dichloride,

[0944] Dimethylsilylenebis(methylcyclopentadienyl)zirconium dichloride,

[0945] Dimethylsilylenebis(dimethylcyclopentadienyl)zirconiumdichloride,

[0946] Dimethylsilylenebis(trimethylcyclopentadienyl) zirconiumdichloride,

[0947] Dimethylsilylenebis(indenyl)zirconium dichloride,

[0948] Dimethylsilylenebis(2-methylindenyl)zirconium dichloride,

[0949] Dimethylsilylenebis(2-methyl, 4-isopropylindenyl)zirconiumdichloride,

[0950] Dimethylsilylenebis(indenyl)zirconiumbis(trifluoromethane-sulfonate),

[0951] Dimethylsilylenebis(4,5,6,7-tetrahydroindenyl)zirconiumdichloride,

[0952] Dimethylsilylene(cyclopentadienyl-fluorenyl)zirconium dichloride,

[0953] Diphenylsilylenebis(indenyl)zirconium dichloride,

[0954] Diphenylsilylenebis(2-methyl, 4-isopropylindenyl)zirconiumdichloride,

[0955] Methylphenylsilylenebis(indenyl)zirconium dichloride,

[0956] Bis(cyclopentadienyl)zirconium dichloride,

[0957] Bis(cyclopentadienyl)zirconium dibromide,

[0958] Bis(cyclopentadienyl)methylzirconium monochloride,

[0959] Bis(cyclopentadienyl)ethylzirconium monochloride,

[0960] Bis(cyclopentadienyl)cyclohexylzirconium monochloride,

[0961] Bis(cyclopentadienyl)phenylzirconium monochloride,

[0962] Bis(cyclopentadienyl)benzylzirconium monochloride,

[0963] Bis(cyclopentadienyl)zirconium monochloride monohydride,

[0964] Bis(cyclopentadienyl)methylzirconium monohydride,

[0965] Bis(cyclopentadienyl)dimethylzirconium,

[0966] Bis(cyclopentadienyl)diphenylzirconium,

[0967] Bis(cyclopentadienyl)dibenzylzirconium,

[0968] Bis(cyclopentadienyl)zirconium methoxychloride,

[0969] Bis(cyclopentadienyl)zirconium ethoxychloride,

[0970] Bis(cyclopentadienyl)zirconium bis(methanesulfonate),

[0971] Bis(cyclopentadienyl)zirconium bis(p-toluenesulfonate),

[0972] Bis(cyclopentadienyl)zirconium bis(trifluoromethanesulfonate),

[0973] Bis(methylcyclopentadienyl)zirconium dichloride,

[0974] Bis(dimethylcyclopentadienyl)zirconium dichloride,

[0975] Bis(dimethylcyclopentadienyl)zirconium ethoxychloride,

[0976] Bis(dimethylcyclopentadienyl)zirconiumbis(trifluoromethanesulfonate),

[0977] Bis (ethylcyclopentadienyl) zirconium dichloride,

[0978] Bis(methylethylcyclopentadienyl)zirconium dichloride,

[0979] Bis(propyl cyclopentadienyl)zirconium dichloride,

[0980] Bis(methylpropylcyclopentadienyl)zirconium dichloride,

[0981] Bis(butylcyclopentadiehyll)zirconium dichloride,

[0982] Bis(methylbutylcyclopentadienyl)zirconium dichloride,

[0983] Bis(methylbutylcyclopentadienyl)zirconium bis(methanesulfonate),

[0984] Bis(trimethylcyclopentadienyl)zirconium dichloride,

[0985] Bis(tetramethylcyclopentadienyl)zirconium dichloride,

[0986] Bis(pentamethylcyclopentadienyl)zirconium dichloride,

[0987] Bis(hexylcyclopentadienyl)zirconium dichloride, and

[0988] Bis(trimethylsilylcyclopetnadienyl)zirconium dichloride.

[0989] In the compounds exemplified above, the di-substitutedcyclopentadienyl ring includes 1,2- and 1,3-substituted compounds, andthe tri-substituted cyclopentadienyl ring includes 1,2,3- and1,2,4-substituted compounds. Further, the alkyl group such as propyl orbutyl includes isomer such as n-, i-, sec-, tert-compounds, In thepresent invention, the above-exemplified zirconium compounds in whichthe zirconium has been replaced by titanium, hafnium, vanadium, niobium,tantalum or chromium can also be used as the transition metal compounds.

[0990] Of the above-exemplified transition metal compounds, preferablyused are the zirconocene compounds which have zirconium as the centralmetal atom and have at least two ligands containing a cyclopentadienylskeleton.

[0991] In the present invention, the transition metal compoundrepresented by the aforementioned formula (I) is particularly preferablyused as the transition metal compound (f).

[0992] The transition metal compounds may be used singly or incombination of two or more kinds. These compounds may be used bydiluting them with hydrocarbons or halogenated hydrocarbons.

[0993] The transition metal compound (f) may be supported on aparticulate carrier. As the carrier, the same particulate carrier asused in the preparation of the olefin polymerization catalyst (2) can bementioned.

[0994] The organoaluminum oxy-compound (b) is identical with theaforesaid organoaluminum oxy-compound, and this organoaluminumoxy-compound (b) can be used by supporting it on the above-mentionedcarrier.

[0995] The compound (g) which reacts with the transition metal compound(f) to form an ion pair is identical with the aforesaid compound (c),and this compound (g) can be used by supporting it on theabove-mentioned carrier.

[0996] The olefin polymerization catalyst (3) used for preparing theethylene/olefin random copolymer (C) can be prepared by mixing thetransition metal compound (f) [component (f)] and the organoaluminumoxy-compound (b) [component (b)] (or the compound (g) which reacts withthe transition metal compound (f) to form an ion pair, [component (g)]),and if desired, the organometallic compound (e) [component (e)) in aninert hydrocarbon solvent or an olefin solvent.

[0997] As the inert hydrocarbon solvent used for the olefinpolymerization catalyst (3), the same inert hydrocarbon solvent as usedfor preparing the olefin polymerization catalyst (1) can be mentioned.

[0998] In the preparation of the olefin polymerization catalyst (3),each components may be mixed in an optional order, but preferably theyare mixed in the following manner:

[0999] the component (b) [or the component (g)] is mixed with thecomponent (f);

[1000] the component (b) is mixed with the component (e), and theresulting mixture is then mixed with the component (f);

[1001] the component (f) is mixed with the component (b) [or

[1002] the component (g)], and the resulting mixture is then mixed withthe component (e); or

[1003] the component (f) is mixed with the component (e), and theresulting mixture is then mixed with the component (b) [or the component(g)].

[1004] In the mixing of each components, an atomic ratio (Al/transitionmetal) of the aluminum in the component (b) to the transition metal inthe component (f) is in the range of usually 10 to 10,000, preferably 20to 5,000; and a concentration of the component (f) is in the range ofabout 10⁻⁸ to 10⁻¹ mol/1-solvent, preferably 10⁻⁷ to 5×10-2mol/1-solvent.

[1005] When the component (g) is used, a molar ratio [component(f)/component (g)] of the component (f) to the component (g) is in therange of usually 0.01 to 10, preferably 0.1 to 5; and a concentration ofthe component (f) is in the range of about 10⁻⁸ to 10⁻¹ mol/1-solvent,preferably 10⁻⁷ to 5×10⁻² mol/1-solvent.

[1006] When the component (e) is used, an atomic ratio (M/A1) of themetal atom (M) in the component (e) to the aluminum atom (Al) in thecomponent (b) is in the range of usually 0.02 to 20, preferably 0.2 to10.

[1007] The above-mentioned components may be mixed in a polymerizer.Otherwise, a mixture of the components beforehand prepared may be fed toa polymerizer.

[1008] If the components are beforehand mixed, the mixing temperature isin the range of usually −50 to 150° C., preferably −2.0 to 120° C.; andthe contact time is in the range of 1 to 1,000 minutes, preferably 5 to600 minutes. The mixing temperature may be varied while the componentsare mixed and contacted with each other.

[1009] The olefin polymerization catalyst (3) may be an olefinpolymerization solid catalyst in which at least one of the component(f), the component (b) [or the component (g)] and the component (e) issupported on an inorganic or organic carrier of granular or particulatesolid.

[1010] As the particulate carrier, those used for the preparation of theaforesaid olefin polymerization catalyst (2) can be employed.

[1011] The olefin polymerization catalyst (3) may be a prepolymerizedcatalyst formed from the particulate carrier, the component (f), thecomponent (b) [or the component (g)] and an olefin polymer produced bythe prepolymerization, and if desired, the component (e).

[1012] The olefin used for the prepolymerization includes olefins suchas propylene, ethylene and 1-butene, but a mixture of these olefins andother olefin may also be employed.

[1013] In addition to the above components, the olefin polymerizationcatalyst (3) may contain other components which are useful for theolefin polymerization, for example, water as a catalyst component.

[1014] The ethylene/olefin random copolymer (C) can be prepared bycopolymerizing ethylene and at least one monomer (olefin) selected fromα-olefins of 3 to 20 carbon atoms and polyenes of 5 to 20 carbon atomsin the presence of the olefin polymerization catalyst (3). In thecopolymerization, ethylene and the olefin are used in such amounts thatthe resulting ethylene/olefin random copolymer (C) has theaforementioned composition.

[1015] The copolymerization to prepare the ethylene/olefin randomcopolymer (C) may be carried out in the presence of a hydrocarbonmedium. Examples of the hydrocarbon media include hydrocarbons which areused for preparing the organoaluminum oxy-compound (b).

[1016] Of such hydrocarbons, preferably used are hexane, methylpentane,methylcyclopentane, heptane, octane, cyclohexane, etc. Also employableas the hydrocarbon medium is an α-olefin which is liquid under thecopolymerization conditions.

[1017] The polymerization of ethylene and an olefin is carried out underthe conditions of a temperature of usually −20 to 200° C., preferably 0to 180° C., particularly preferably 20 to 160° C., and a pressure ofusually atmospheric pressure to 100 kg/cm², preferably atmosphericpressure to 50 kg/cm², particularly preferably atmospheric pressure to30 kg/cm².

[1018] The molecular weight of the resulting copolymer can be regulatedby varying the polymerization conditions such as a polymerizationtemperature or by controlling the amount of hydrogen (molecular weightregulator) used.

[1019] In the present invention, the molecular weight is regulated sothat the resulting copolymer has MFR of the aforesaid value.

[1020] The copolymerization may be carried out by a solutionpolymerization process, a suspension polymerization process, etc. Inthis invention, a solution polymerization process is preferably used.Though the polymerization reaction may be carried out either batchwise,semi-continuously or continuously, it is preferably carried outcontinuously. Further, it is also possible to conduct the polymerizationin two or more steps having different reaction conditions.

[1021] The polymer obtained immediately after the polymerization can berecovered by conventionally known separation and recovery methods.

[1022] In the case of the solution polymerization, it is preferred tosolidify the polymer by directly evaporating the solvent, or to solidifythe polymer by evaporating the solvent from the concentrated phase afterphase separation.

The Sixth Propylene Polymer Composition

[1023] The sixth propylene polymer composition comprises:

[1024] (A5) a propylene homopolymer which is obtain-ed by polymerizingpropylene in the presence of an olefin polymerization catalystcomprising:

[1025] (i) (h) a transition metal compound represented by the aforesaidformula (I), and

[1026] (ii) at least one compound selected from the group consisting of

[1027] (b) an organoaluminum oxy-compound, and

[1028] (i) a compound which reacts with the transition metal compound(h) to form an ion pair; and

[1029] (A6) a propylene polymer which contains constituent units derivedfrom propylene in an amount of not less than 90% by mol and is differentfrom the propylene homopolymer (A5).

[1030] Propylene Homopolymer (A5)

[1031] The propylene homopolymer (A5) for constituting thesixth-propylene polymer composition is a homopolymer of propylene whichis prepared by the use of an olefin polymerization catalyst comprising atransition metal compound (h) represented by the aforesaid formula (I)and at least one compound selected from the organoaluminum oxy-compound(b) and the compound (i).

[1032] The propylene homopolymer (A5) is desired to have MFR, asmeasured at 230° C. under a load of 2.16 kg, of 0.01 to 1,000 g/10 min,preferably 0.5 to 200 g/10 min, and Mw/Mn, as measured by GPC, of 1.5 to3.5, preferably 2.0 to 3.0, more preferably 2.0 to 2.5.

[1033] Further, the propylene homopolymer (A5) is desired to have anintrinsic viscosity [11, as measured in decalin at 135° C., of 0.1 to 20dl/g, preferably 0.5 to 10 dl/g, more preferably 1 to 5 dl/g, and aweight-average molecular weight of 1×10³ to 500×10⁴, preferably 1×10⁴ to100×10⁴.

[1034] The crystallinity of the propylene homopolymer (A5), as measuredby X-ray diffractometry, is desired to be not less than 40%, preferablynot less than 50%, and the boiling heptane extraction residue proportion(I.I.) thereof is desired to be not less than 90%, preferably not lessthan 93%.

[1035] The triad tacticity (mm fraction) of the propylene homopolymer(A5) is desired to be not less than 99.0%, preferably not less than99.2%, more preferably not less than 99.5%.

[1036] The proportion of the irregularly positioned units (inverselyinserted units) based on the 2,1-insertion of the propylene monomer isdesired to be not more than 0.5%, preferably not more than 0.18%, morepreferably not more than 0.15%.

[1037] The proportion of the irregularly positioned units based on the1,3-insertion of the propylene monomer is desired to be less than thedetected lower limit by the ¹³C-NMR measurement (less than 0.03%)

[1038] The triad tacticity (mm fraction), the proportion of theirregularly positioned units based on the 2,1-insertion of the propylenemonomer, and the proportion of the irregularly positioned units based onthe 1,3-insertion of the propylene monomer, of the above-mentionedpropylene homopolymer and the later-described propylene copolymer aredetermined in the following manner.

[1039] [Triad Tacticity (mm Fraction)]

[1040] The triad tacticity (mm fraction) of the propylene copolymer isdefined, when a sequence of optional three propylene units withhead-to-tail bonds in the polymer chain is expressed by a planar zigzagstructure, as a proportion of such propylene unit sequences that thedirection of methyl branches thereof are the same as each other, anddetermined by the ¹³C-NMR spectrum using the following equation:${{Triad}\quad {tacticity}\quad (\%)} = {\frac{{PPP}\quad ({mm})}{{{PPP}\quad ({mm})} + {{PPP}\quad ({mr})} + {{PPP}\quad ({rr})}} \times 100}$

[1041] wherein PPP (mm), PPP(mr) and PPP(rr) denote absorptionintensities originating from the methyl group of the second unit in the3-propylene unit sequences with head-to-tail bonds represented by thefollowing formulas, respectively:

[1042] The ¹³C-NMR spectrum was measured in the following manner. Asample was completely dissolved in a mixed solvent containing about 0.5ml of hexachlorobutadiene, o-dichlorobenzene or 1,2,4-trichlorobenzeneand about 0.05 ml of deuterated benzene (i.e., lock solvent) in a NMRsample tube (diameter: 5 mm), and then subjected to a proton perfectdecoupling method at 120° C. to measure the ¹³C-NMR spectrum. Themeasurement is conducted under the conditions of a flip angle of 45° anda pulse interval of not less than 3.4 T₁ (T₁ is a maximum value withrespect to a spin-lattice relaxation time of the methyl group). As forthe propylene, the spin-lattice relaxation time of the methyl group islonger than that of the methylene group and that of the methine group,and hence the magnetization recovery of all carbons in the sample underthese conditions is not less than 99%. With respect to the chemicalshift, the methyl group of the third unit in the 5-propylene unitsequence with head-to-tail bonds is set to 21.593 ppm, and the chemicalshift of other carbon peak is determined by using this value as areference.

[1043] The peak region is classified into the first region (21.1-21.9ppm), the second region (20.3-21.0 ppm) and the third region (19.5-20.3ppm).

[1044] In the first region, the methyl group of the second unit in the3-propylene unit sequence represented by PPP (mm) resonates.

[1045] In the second region, the methyl group of the second unit in the3-propylene unit sequence represented by PPP(mr) and the methyl group(PPE-methyl group) of a propylene unit whose adjacent units are apropylene unit and an ethylene unit resonate.

[1046] In the third region, the methyl group of the second unit in the3-propylene unit sequence represented by PPP(rr) and the methyl group(EPE-methyl group) of a propylene unit whose adjacent units are ethyleneunits resonate.

[1047] The propylene copolymer has, as partial structures containing anirregularly positioned unit, the following structures (i), (ii) and(iii):

[1048] Of the peaks originating from these structures (i), (ii) and(iii), the peaks based on the carbon A and the carbon B do not appear inthe first to third regions, because the carbon A and the carbon Bresonate at 17.3 ppm and 17.0 ppm, respectively. Further, the carbon Aand the carbon B have no concern with the 3-propylene unit sequence withhead-to-tail bonds, so that it is unnecessary to take those carbons intoaccount in the calculation of the triad tacticity.

[1049] The peak based on the carbon C, the peak based on the carbon Dand the peak based on the carbon D′ appear in the second region, and thepeak based on the carbon E and the peak based on the carbon E appear inthe third region.

[1050] Accordingly, of the peaks which appear in the first to thirdregions, the peaks which are not based on the 3-propylene unit sequencewith heat-to-tail bonds are those based on the PPE-methyl group(resonance in the vicinity of 20.7 ppm), the EPE-methyl group (resonancein the vicinity of 19.8 ppm), the carbon C, the carbon D, the carbon D′,the carbon E and the carbon E′.

[1051] The peak area based on the PPE-methyl group can be determinedfrom the peak area of the PPE-methine group (resonance in the vicinityof 30.6 ppm); and the peak area based on the EPE-methyl group can bedetermined from the peak area of the EPE methine group (resonance in thevicinity of 32.9 ppm). The peak area based on the carbon C can bedetermined from the peak area of the adjacent methine group (resonancein the vicinity of 31.3 ppm); the peak area based on the carbon D can bedetermined from 1/2 as much as the sum of the peak areas of the peaksbased on the αβ methylene carbons of the above structure (ii) (resonancein the vicinity of the 34.3 ppm and in the vicinity of 34.5 ppm); thepeak area based on the carbon D′ can be determined from the peak areabased on the methine group adjacent to the methyl group (resonance inthe vicinity of 33.3 ppm) of the carbon E′ of the above structure (iii);the peak area based on the carbon E can be determined from the peak areaof the adjacent methine carbon (resonance in the vicinity of 33.7 ppm);and the peak area based on the carbon E′ can be determined from the peakarea of the adjacent methine carbon (resonance in the vicinity of 33.3ppm).

[1052] Accordingly, by subtracting these peak areas from the total peakareas of the second and third regions, the peak areas originating fromthe 3-propylene unit sequences (PPP(mr) and PPP(rr)) consisting ofhead-to-tail bonds can be obtained.

[1053] Thus, the peak areas of PPP(mm), PPP(mr) and PPP(rr) can bedetermined, and hence the triad tacticity (mm fraction) of the propyleneunit sequences consisting of the head-to-tail bonds can be calculated bythe above-mentioned equation.

[1054] The triad tacticity (mm fraction) of the propylene homopolymer isdefined, when a sequence of optional three propylene units withhead-to-tail bonds in the polymer chain is expressed by a planar zigzagstructure, as a proportion of such propylene unit sequences that thedirection of methyl groups thereof are the same as each other, anddetermined by the ¹³C-NMR spectrum using the following equation:${{Triad}\quad {tacticity}\quad (\%)} = \frac{{PPP}\quad ({mm})}{\Sigma \quad {ICH}_{3}}$

[1055] wherein PPP(mm) has the same meaning as defined above, and ΣICH₃denotes the total peak areas based on all of the methyl groups.

[1056] With respect, to the chemical shift, the methyl group of thethird unit in the 5-propylene unit sequence with heat-to-tail bonds isset to 21.593 ppm, and the chemical shift of other carbon peak isdetermined by using this value as a standard.

[1057] In accordance with the standard, the peak based on the methylgroup of the second unit in the 3-propylene unit sequence represented byPPP(mm) appears within the range of 21.1 to 21.9 ppm; the peak based onthe methyl group of the second unit in the 3-propylene unit sequencerepresented by PPP(mr) appears within the range of 20.3 to 21.0 ppm; andthe peak based on the methyl group of the second unit in the 3-propyleneunit sequence represented by PPP(rr) appears within the range of 19.5 to20.3 ppm.

[1058] The propylene homopolymer has such a partial structure containingthe irregularly positioned unit based on the 2,1-insertion asrepresented by the aforesaid structure (i) in a small amount, inaddition to the regular structure in which the propylene units arebonding with head-to-tail.

[1059] In the irregular structure represented by the structure (i), theaforementioned definition of PPP(mm) is not applied to the carbon A, thecarbon B and the carbon C. However, the carbon A and the carbon Bresonate in the region of 16.5 to 17.5 ppm; and the carbon C resonatesin the vicinity of 20.7 ppm (the region of PPP(mr)). (However, not onlythe peaks of these methyl groups but also the peaks of the adjacentmethylene and methine groups must be confirmed in the case ofidentifying the partial structure containing an irregularly positionedunit.) Therefore, the carbon A, the carbon B and the carbon C are notincluded in the region of PPP(mm).

[1060] Accordingly, the triad tacticity (mm fraction) of the propylenehomopolymer can be determined from the above equation.

[1061] [Proportion of the irregularly positioned unit based on the2,1-insertion of the propylene monomer]In the polymerization, the1,2-insertion of the propylene monomer often takes place (i.e., themethylene side is bonded to the catalyst), but the 2,1-insertion thereofsometimes takes place. Therefore, the propylene copolymer has suchirregularly positioned units based on the 2,1-insertion as representedby the aforesaid structures (i), (ii) and (iii). The proportion of theirregularly positioned units based on the 2,1-insertion was calculatedby the following formula using the ¹³C-NMR. $\begin{matrix}{{{Proportion}\quad {of}\quad {irregularly}\quad {positioned}\quad {unit}\quad {based}\quad {on}\quad 2},{{1\text{-}{insertion}} =}} \\{\quad \frac{\{ {{0.5\quad I\quad \alpha \quad {\beta ( {{{structure}\quad (i)},({iii})} )}} + {0.25\quad I\quad \alpha \quad {\beta ( {{structure}\quad ({ii})} )}}} \} \times 100}{{I\quad \alpha \quad \alpha} + {I\quad \alpha \quad {\beta ( {{{structure}\quad (i)},({iii})} )}} + {0.5( {{I\quad \alpha \quad \gamma} + {I\quad \alpha \quad {\beta ( {{{structure}\quad ({ii})} + {I\quad \alpha \quad \delta}} )}}} }}}\end{matrix}$

[1062] Naming of the peaks was made in accordance with a method byCarman, et al. (Rubber Chem. Technol., 44 (1971), 781). I_(αβ) denotes apeak area of the αβ peak.

[1063] The propylene homopolymer has such an irregularly positioned unitbased on the 2,1-insertion as represented by the aforesaid structure(i). The proportion of the irregularly positioned units based on the2,1-insertion was calculated by the following formula using the ¹³C-NMR.${{Proportion}\quad {of}\quad {irregularly}\quad {positioned}\quad {unit}\quad {based}\quad {on}\quad 2},{{1\text{-}{insertion}} = \text{}\frac{\begin{matrix}{0.5\{ {{area}\quad {based}\quad {on}\quad {methyl}\quad {group}\quad {resonating}\quad {in}\quad {the}\quad {region}\quad {of}} } \\ {16.5 \sim {17.5\quad {ppm}}} \}\end{matrix}}{\Sigma \quad {ICH}_{3}}}$

[1064] wherein ΣICH₃ has the same meaning as defined above.

[1065] [Proportion of the Irregularly Positioned Unit Based on the1,3-Insertion of the Propylene Monomer]

[1066] In the propylene copolymer, the amount of the three sequencesbased on the 1,3-insertion of propylene was determined by the βy peak(resonance in the vicinity of 27.4 ppm).

[1067] In the propylene homopolymer, the amount of the three sequencesbased on the 1,3-insertion of propylene was determined by the αδ peak(resonance in the vicinity of 37.1 ppm) and the βy peak (resonance inthe vicinity of 27.4 ppm).

[1068] Propylene Polymer (A6)

[1069] The propylene polymer (A6) is a propylene homopolymer or apropylene copolymer containing constituent units derived from propylenein an amount of not less than 90% by mol.

[1070] The propylene polymer (A6) is desired to have MFR, as measured at230° C. under a load of 2.16 kg, of 0.01 to 1,000 g/10 min, preferably0.5 to 200 g/10 min. The molecular weight distribution (Mw/Mn) of thispropylene polymer, as measured by GPC, is desired to be in the range of1.5 to 15, preferably 2.0 to 8.0.

[1071] Further, the propylene polymer (A6) is desired to have acrystallinity, as measured by X-ray diffractometry, of not less than40%, more preferably not less than 50%.

[1072] The propylene polymer (A6) is desired to have an intrinsicviscosity [η], as measured in decalin at 135° C., of 0.1 to 20 dl/g,preferably 0.5 to 10 dl/g, and a weight-average molecular weight of1×10³ to 500×10⁴, preferably 1×10⁴ to 100×10⁴.

[1073] The propylene polymer (A6) may contain constituent units derivedfrom ethylene and the same α-olefins of 4 to 20 carbon atoms asexemplified for the propylene polymer (A4) in the amounts of not morethan 10%.

[1074] The propylene polymer (A6) can be prepared by the use of theolefin polymerization catalyst which is used for preparing the propylenepolymer (A1), the olefin polymerization catalyst (2) which is used forpreparing the propylene polymer (A3), the olefin polymerization catalyst(3) which is used for preparing the ethylene/α-olefin random copolymer(C), or an olefin polymerization catalyst (4) (described later) which isused for preparing the propylene polymer (A5). Among these olefinpolymerization catalysts, preferably used are the olefin polymerizationcatalyst (1), the olefin polymerization catalyst (3) and the olefinpolymerization catalyst (4), and of these, particularly preferably usedis the olefin polymerization catalyst (4).

[1075] Propylene Polymer Composition

[1076] The sixth propylene polymer composition comprises the propylenehomopolymer (A5) and the propylene polymer (A6) which is different fromthe propylene homopolymer (A5). In this composition, it is desired thatthe propylene homopolymer (A5) is contained in an amount of 5 to 95% byweight, preferably 15 to 85% by weight, more preferably 30 to 70% byweight; and the propylene polymer (A6) is contained in an amount of 5 to95% by weight, preferably 15 to 85% by weight, more preferably 30 to 70%by weight.

[1077] In the sixth propylene polymer composition, when the intrinsicviscosity ([η]_(A5)) of the propylene homopolymer (A5) and the intrinsicviscosity ([η]_(A6)) of the propylene polymer (A6) has a relation of[η]_(A5)≧([η]_(A6) it is desired that [η]_(A)5 is in the range of 1 to10 dl/g, preferably 2 to 5 dl/g; ([η]_(A6) is in the range of 0.2 to 1.5dl/g, preferably 0.3 to 1.0 dl/g; and ([η]_(A5)/[η]_(A6)) is in therange of 3 to 30, preferably 4 to 20.

[1078] When the intrinsic viscosity ([η]_(A5)) of the propylenehomopolymer (A5) and the intrinsic viscosity ([η]_(A6)) of the propylenepolymer (A6) has a relation of [η]_(A5)<[η]_(A6)′ it is desired that[η]_(A5) is in the range of 0.2 to 1.5 dl/g, preferably 0.3 to 1.0 dl/g;[η]_(A6) is in the range of 1 to 10 dl/g, preferably 2 to 5 dl/g; and([η]_(A6/)/[η]_(A5)) is in the range of 3 to 30, preferably 4 to 20.

[1079] The sixth propylene polymer composition is desired to have MFR,as measured at 230° C. under a load of 2.16 kg, of 0.01 to 1,000 g/10min, preferably 0.5 to 200 g/10 min. In this composition, Mw/Mn of allthe propylene components for constituting the composition is desirablyin the range of 4 to 15.

[1080] The density of the sixth propylene polymer composition is desiredto be in the range of 0.89 to 0.92 g/cm³, preferably 0.90 to 0.92 g/cm³.

[1081] The flexural modulus (FM) thereof is desired to be in the rangeof 12,000 to 21,000 kg/cm², preferably 14,000 to 20,000 kg/cm².

[1082] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 2 to 10 kg·cm/cm, preferably 2 to 5 kg·cm/cm.

[1083] The tensile elongation at break (EL) thereof is desired to be inthe range of 100 to 500%, preferably 200 to 400%. The heat distortiontemperature (HDT) thereof is desired to be not lower than 95° C.,preferably in the range of 100 to 140° C.

[1084] The sixth propylene polymer composition may contain, ifnecessary, additives which may be added to the first propylene polymercomposition, with the proviso that the object of the invention is notmarred.

[1085] The sixth propylene polymer composition can be prepared by knownprocesses. For example, the composition can be prepared in accordancewith the processes (1) to (5) described for the first propylene polymercomposition, using the propylene homopolymer (A5) and the propylenepolymer (A6).

[1086] Such sixth propylene polymer composition is excellent in not onlyheat resistance, rigidity and tensile elongation at break but alsomoldability.

[1087] The sixth propylene polymer composition can be favorably used forvarious structural materials such as those of automobiles and electricalappliances, daily necessaries, various films and sheets.

[1088] Next, the catalyst used for the preparation of the propylenepolymer (A5) and the process for preparing the propylene homopolymer aredescribed.

[1089] The olefin polymerization catalyst used for preparing thepropylene homopolymer (A5) is an olefin polymerization catalyst [olefinpolymerization catalyst (4)] comprising:

[1090] (i) (h) a transition metal compound represented by the aforesaidformula (I), and

[1091] (ii) at least one compound selected from the group consisting of

[1092] (b) the organoaluminum oxy-compound, and

[1093] (i) a compound which reacts with the transition metal compound(h) to form an ion pair.

[1094]FIG. 4 illustrates steps of a process for preparing the olefinpolymerization catalyst which is used for the preparation of thepropylene homopolymer (A5).

[1095] The compound (i) which reacts with the transition metal compound(h) to form an ion pair is identical with the compound (c) which reactswith the transition metal compound (a) to form an ion pair.

[1096] The compound (i) which reacts with the transition metal compound(h) to form an ion pair can be used in combination of two or more kinds.

[1097] The olefin polymerization catalyst used for the preparation ofthe propylene homopolymer (A5) may contain the aforesaid organoaluminumcompound (j) in addition to the transition metal compound (h) and atleast one compound selected from the group consisting of theorganoaluminum oxy-compound (b) and the compound (i).

[1098] The olefin polymerization catalyst (4) can be prepared by mixingthe transition metal compound (h) (component (h)] and the organoaluminumoxy-compound (b) [component (b)] (or the compound (i) which reacts withthe transition metal compound (h) to form an ion pair, [component (i)]),and if desired, the organoaluminum compound (j) [component (j)] in aninert hydrocarbon solvent or an olefin solvent.

[1099] As the inert hydrocarbon solvent used for preparing the catalyst,the same inert hydrocarbon solvent as used for preparing the olefinpolymerization catalyst (1) can be employed.

[1100] In the preparation of the olefin polymerization catalyst (4),each components may be mixed in an optional order, but preferably theyare mixed in the following manner:

[1101] the component (b) (or the component (i)] is mixed with thecomponent (h);

[1102] the component (b) is mixed with the component (j), and theresulting mixture is then mixed with the component (h);

[1103] the. component (h) is mixed with the component (b) [or thecomponent (i)), and the resulting mixture is then mixed with thecomponent (j); or

[1104] the component (h) is mixed with the component (j), and theresulting mixture is then mixed with the component (b) [or the component(i)].

[1105] In the mixing of each components, an atomic ratio (Al/transitionmetal) of the aluminum in the component (b) to the transition metal inthe component (h) is in the range of usually 10 to 10,000, preferably 20to 5,000; and a concentration of the component (h) is in the range ofabout 10⁻⁸ to 10⁻¹ mol/1-solvent, preferably 10⁻⁷ to 5×10⁻²mol/1-solvent.

[1106] When the component (i) is used, a molar ratio [component(h)/component (i)] of the component (h) to the component (i) is in therange of usually 0.01 to 10, preferably 0.1 to 5; and a concentration ofthe component (h) is in the range of about 10⁻⁸ to 10⁻¹ mol/1-solvent,preferably 10⁻⁷ to 5×10⁻² mol/1-solvent.

[1107] When the component (j) is used, an atomic ratio (Al_(j)/Al_(b))of the aluminum atom (Al_(j)) in the component (j) to the aluminum atom(Al_(b)) in the component (b) is in the range of usually 0.02 to 20,preferably 0.2 to 10.

[1108] The above-mentioned components may be mixed in a polymerizer.Otherwise, a mixture of the components beforehand prepared may be fed toa polymerizer.

[1109] If the components are beforehand mixed, the mixing temperature isin the range of usually −50 to 150° C., preferably −20 to 120° C.; andthe contact time is in the range of 1 to 1,000 minutes, preferably 5 to600 minutes. The mixing temperature may be varied while the componentsare mixed and contacted with each other.

[1110] The olefin polymerization catalyst (4) may be an olefinpolymerization catalyst in which at least one of the component (h), thecomponent (b) [or the component (i)] and the component (j) is supportedon an inorganic or organic carrier of granular or particulate solid.

[1111] The inorganic carrier is preferably a porous oxide, for example,SiO₂ or Al₂O₃.

[1112] Examples of the granular or particulate solid organic compoundsinclude polymers or copolymers produced mainly from α-olefins such asethylene, propylene and 1-butene or styrene.

[1113] The olefin polymerization catalyst (4) may be an olefinpolymerization catalyst formed from the particulate carrier, thecomponent (h), the component (b) [or the component (i)] and an olefinpolymer prepared by prepolymerization, and if desired, the component(j).

[1114] The olefin used for the prepolymerization includes olefins suchas propylene, ethylene and 1-butene, but a mixture of these olefins andother olefin may also be employed.

[1115] In addition to the above components, the olefin polymerizationcatalyst (4) may contain other components which are useful for theolefin polymerization, for example, water as a catalyst component.

[1116] The propylene homopolymer (A5) can be prepared by polymerizingpropylene in the presence of the olefin polymerization catalyst (4). Thepolymerization may be carried out by either a liquid phasepolymerization process such as a suspension polymerization process and asolution polymerization process, or a gas phase polymerization process.

[1117] In the liquid phase polymerization process, the same inerthydrocarbon solvent as used in the preparation of the catalyst describedbefore can be used, or propylene can be also used as a solvent.

[1118] In the suspension polymerization process, the temperature forpolymerizing propylene is in the range of usually −50 to 100° C.,preferably 0 to 90° C. In the solution polymerization process, thepolymerization temperature is in the range of usually 0 to 250° C.,preferably 20 to 200° C. In the gas phase polymerization process, thepolymerization temperature is in the range of usually 0 to 120° C.,preferably 20 to 100° C. The polymerization pressure is in the range ofusually atmospheric pressure to 100 kg/cm², preferably atmosphericpressure to 50 kg/cm². The polymerization reaction may be carried outeither batchwise, semi-continuously or continuously. Further, it is alsopossible to conduct the polymerization in two or more steps havingdifferent reaction conditions.

The Seventh Propylene Polymer Composition

[1119] The seventh propylene polymer composition of the inventioncomprises:

[1120] (A5) a propylene homopolymer which is obtained by polymerizingpropylene in the presence of an olefin polymerization catalystcomprising:

[1121] (i) (h) a transition metal compound represented by the aforesaidformula (I), and

[1122] (ii) at least one compound selected from the group consisting of

[1123] (b) an organoaluminum oxy-compound, and

[1124] (i) a compound which reacts with the transition metal compound(h) to form an ion pair; and

[1125] (D) an olefin elastomer which is characterized in that:

[1126] (1) the elastomer is obtained by polymerizing or copolymerizingat least one monomer selected from olefins of 2 to 20 carbon atoms andpolyenes of 5 to 20 carbon atoms,

[1127] (2) the elastomer contains constituent units derived fromethylene, propylene, butene or 4-methyl-1-pentene in an amount of lessthan 90% by mol, and

[1128] (3) the elastomer has a glass transition temperature (Tg) of nothigher than 10° C.

[1129] Propylene Homopolymer (A5)

[1130] The propylene homopolymer (A5) for constituting the seventhpropylene polymer composition is identical with the propylenehomopolymer (A5) for constituting the sixth propylene polymercomposition.

[1131] Olefin Elastomer (D)

[1132] The olefin elastomer (D) is a polymer of one monomer selectedfrom the group consisting of olefins of 2 to 20 carbon atoms andpolyenes of 5 to 20 carbon atoms, or a random or block copolymer of twoor more monomers selected from olefins of 2 to 20 carbon atoms andpolyenes of 5 to 20 carbon atoms. This olefin elastomer (D) contains[constituent units derived from ethylene, propylene, butene or4-methyl-1-pentene in an amount of less than 90%, preferably not morethan 85%, and has a glass transition temperature (Tg) of not higher than10° C., preferably −100 to 0° C., more preferably −100 to −10° C.

[1133] Examples of the olefins of 2 to 20 carbon atoms include ethylene,propylene, 1-butene, 1-pentene, 2-methyl-1-butene, 3-methyl-1-butene,1-hexene, 3-methyl-1-pentene, 4-methyl-1-pentene, 3,3-dimethyl-1-butene,1-heptene, methyl-1-hexene, dimethyl-1-pentene, trimethyl-1-butene,ethyl-1-pentene, 1-octene, methyl-1-pentene, dimethyl-1-hexene,trimethyl-1-pentene, ethyl-1-hexene, methylethyl-1-pentene,diethyl-1-butene, propyl-1-pentene, 1-decene, methyl-1-nonene,dimethyl-1-octene, trimethyl-1-heptene, ethyl-1-octene,methylethyl-1-heptene, diethyl-1-hexene, 1-dodecene, hexadodecene andstyrene.

[1134] Examples of the polyenes of 5 to 20 carbon atoms include polyenesexemplified for the ethylene/olefin random polymer (C).

[1135] Such olefin elastomer (D) is desired to have a density of 0.85 to0.92 g/cm³, preferably 0.85 to 0.90 g/cm³, and an intrinsic viscosity[η], as measured in decalin at 135° C., of 0.1 to 20 dl/g, preferably0.5 to 10 dl/g, more preferably 1 to 5 dl/g.

[1136] Further, the olefin elastomer (D) is desired to have acrystallinity, as measured by X-ray diffractometry, of less than 30% orto be amorphous.

[1137] As the olefin elastomer (D), there can be mentioned, for example,a copolymer of two or more monomers selected from olefins of 2 to 20carbon atoms, a copolymer of one monomer selected from olefins of 2 to20 carbon atoms and one monomer selected from polyenes of 5 to 20 carbonatoms, and a copolymer of two or more monomers selected from olefins of2 to 20 carbon atoms and one monomer selected from polyenes of 5 to 20carbon atoms.

[1138] More specifically, there can be mentioned:

[1139] an elastomer containing constituent units derived from ethylenein an amount of 50 to 90% by mol and constituent units derived from amonomer selected from olefins of 3 to 20 carbon atoms and polyenes of 5to 20 carbon atoms in an amount of 10 to 50% by mol,

[1140] an elastomer containing constituent units derived from ethylenein an amount of 60 to 90% by mol and constituent units derived from amonomer selected from olefins of 3 to 6 carbon atoms and polyenes of 5and 6 carbon atoms in an amount of 10 to 40% by mol;

[1141] an elastomer containing constituent units derived from ethylenein an amount of 65 to 90% by mol and constituent units derived from amonomer selected from propylene and butene in an amount of 10 to 35% bymol;

[1142] an elastomer containing constituent units derived from propylenein an amount of 50 to 90% by mol and constituent units derived from amonomer selected from ethylene, olefins of 4 to 20 carbon atoms andpolyenes of 5 to 20 carbon atoms in an amount of 10 to 50% by mol;

[1143] an elastomer containing constituent units derived from propylenein an amount of 50 to 85% by mol and constituent units derived from amonomer selected from ethylene, olefins of 4 to 6 carbon atoms andpolyenes of 5 and 6 carbon atoms in an amount of 15 to 50% by mol;

[1144] an elastomer containing constituent units derived from propylenein an amount of 50 to 80% by mol and constituent units derived from amonomer selected from ethylene and butene in an amount of 20 to 50% bymol; and

[1145] and others, such as a styrene/butadiene rubber (SBR) and astyrene block copolymer (SEBS) having poly(ethylene-butene) in therubber intermediate block.

[1146] The olefin elastomer (D) can be obtained by polymerizing orcopolymerizing at least one monomer selected from the group consistingof olefins of 2 to 20 carbon atoms and polyenes of 5 to 20 carbon atomsby conventionally known processes. The polymerization reaction can becarried out in a gas phase (gas phase process) or in a liquid phase(liquid phase process).

[1147] The olefin elastomer (D) can be used in combination of two ormore kinds.

[1148] Propylene Polymer Composition

[1149] The seventh propylene polymer composition comprises the propylenehomopolymer (A5) and the olefin elastomer (D). In this composition, itis desired that the propylene homopolymer (AS) is contained in an amountof 5 to 95% by weight, preferably 30 to 90% by weight, more preferably50 to 80% by weight; and the olefin elastomer (D) is contained in anamount of 5 to 95% by weight, preferably 10 to 70% by weight, morepreferably 20 to 50% by weight.

[1150] The seventh propylene polymer composition is desired to have MFR,as measured at 230° C. under a load of 2.16 kg, of 0.01 to 1,000 g/10min, preferably 0.5 to 200 g/10 min. In this composition, Mw/Mn of allthe propylene components for constituting the composition is desirablyin the range of 1.5 to 3.5.

[1151] The density of the seventh propylene polymer composition isdesired to be in the range of 0.88 to 0.92 g/cm³, preferably 0.90 to0.92 g/cm³.

[1152] The flexural modulus (FM) thereof is desired to be in the rangeof 8,000 to 21,000 kg/cm², preferably 12,000 to 20,000 kg/cm².

[1153] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 10 to 60 kg·cm/cm, preferably 10 to 40 kg·cm/cm.

[1154] The tensile elongation at break (EL) thereof is desired to be inthe range of 200 to 1,000%, preferably 300 to 500%.

[1155] The heat distortion temperature (HDT) thereof is desired to benot lower than 85° C., preferably in the range of 95 to 140° C.

[1156] The seventh propylene polymer composition may contain, ifnecessary, additives which may be added to the first propylene polymercomposition, with the proviso that the object of the invention is notmarred.

[1157] The seventh propylene polymer composition can be prepared byknown processes. For example, the composition can be prepared inaccordance with the processes (1) to (5) described for the firstpropylene polymer composition, using the propylene homopolymer (A5) andthe olefin elastomer (D) Such propylene polymer composition is excellentin not only heat resistance, rigidity and tensile elongation at breakbut also impact resistance.

[1158] The seventh propylene polymer composition can be favorably usedfor various structural materials such as those of automobiles andelectrical appliances, daily necessaries and various sheets.

The Eighth Propylene Polymer Composition

[1159] The eighth propylene polymer composition of the inventioncomprises:

[1160] (A5) a propylene homopolymer which is obtained by polymerizingpropylene in the presence of an olefin polymerization catalystcomprising:

[1161] (i) (h) a transition metal compound represented by the aforesaidformula (I), and

[1162] (ii) at least one compound selected from the group consisting of

[1163] (b) an organoaluminum oxy-compound, and

[1164] (i) a compound which reacts with the transition metal compound(h) to form an ion pair; and

[1165] (E) an olefin polymer which contains constituent units derivedfrom one monomer selected from the group consisting of ethylene, buteneand 4-methyl-1-pentene in an amount of not less than 90% by mol.

[1166] Propylene Homopolymer (A5)

[1167] The propylene homopolymer (A5) for constituting the eighthpropylene polymer composition is identical with the propylenehomopolymer (A5) for constituting the sixth propylene polymercomposition.

[1168] Olefin Polymer (E)

[1169] The olefin polymer (E) is either an ethylene (co)polymercontaining constituent units derived from ethylene in an amount of notless than 90% by mol, preferably not less than 95% by mol, a butene(co)polymer containing constituent units derived from butene in anamount of not less than 90% by mol, preferably not less than 95% by mol,or a 4-methyl-1-pentene (co)polymer containing constituent units derivedfrom 4-methyl-1-pentene in an amount of not less than 90% by mol,preferably not less than 95% by mol.

[1170] The ethylene copolymer may contain constituent units derived froma monomer selected from the group consisting of olefins of 3 to 20carbon atoms and polyenes of 5 to 20 carbons atoms in an amount of lessthan 10% by mol.

[1171] The butene copolymer may contain constituent units derived from amonomer selected from the group consisting of other olefins of 2 to 20carbon atoms than butene and polyenes of 5 to 20 carbons atoms in anamount of less than 10% by mol.

[1172] The 4-methyl-1-pentene copolymer may contain constituent unitsderived from a monomer selected from the group consisting of otherolefins of 2 to 20 carbon atoms than 4-methyl-1-pentene and polyenes of5 to 20 carbons atoms in an amount of less than 10% by mol.

[1173] Examples of the olefins of 2 to 20 carbon atoms include olefinsexemplified for the olefin elastomer (D).

[1174] Examples of the polyenes of 5 to 20 carbon atoms include polyenesexemplified for the olefin elastomer (D).

[1175] Such olefin polymer (E) is desired to have a density of 0.80 to0.98 g/cm³, preferably 0.85 to 0.96 g/cm³, and an intrinsic viscosity[η]; as measured in decalin at 135° C., of 0.1 to 20 dl/g, preferably0.5 to 10 dl/g, more preferably 1 to 5 dl/g.

[1176] The olefin polymer (E) is preferably an ethylene homopolymer oran ethylene copolymer, and more preferably an ethylene homopolymer.

[1177] The olefin polymer (E) can be obtained by polymerizing onemonomer selected from the group consisting of ethylene, butene and4-methyl-1-pentene or copolymerizing one monomer selected from the groupconsisting of ethylene, butene and 4-methyl-1-pentene with at least onemonomer selected from other olefins of 2 to 20 carbon atoms than theabove monomers and polyenes of 5 to 20 carbon atoms, in accordance withconventionally known processes. The polymerization reaction can becarried out in a gas phase (gas phase process) or in a liquid phase(liquid phase process).

[1178] The olefin polymer (E) can be used in combination of two or morekinds.

[1179] Propylene Polymer Composition

[1180] The eighth propylene polymer composition comprises the propylenehomopolymer (A5) and the olefin polymer (E). In this composition, it isdesired that the propylene homopolymer (A5) is contained in an amount of5 to 95% by weight, preferably 30 to 90% by weight, more preferably 50to 80% by weight; and the olefin polymer (E) is contained in an amountof 5 to 95% by weight, preferably 10 to 70% by weight, more preferably20 to 50% by weight.

[1181] The eighth propylene polymer composition is desired to have MFR,as measured at 230° C. under a load of 2.16 kg, of 0.1 to 200 g/10 min,preferably 1 to 100 g/10 min. In this composition, Mw/Mn of all thepropylene components for constituting the composition is desirably inthe range of 1.5 to 3.5.

[1182] The density of the eighth propylene polymer composition isdesired to be in the range of 0.80 to 0.98 g/cm³, preferably 0.85 to0.94 g/cm³.

[1183] The flexural modulus (FM) thereof is desired to be in the rangeof 12,000 to 21,000 kg/cm², preferably 14,000 to 20,000 kg/cm².

[1184] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 2 to 20 kg·cm/cm, preferably 2 to 10 kg·cm/cm.

[1185] The tensile elongation at break (EL) thereof is desired to be inthe range of 100 to 500%, preferably 200 to 400%.

[1186] The heat distortion temperature (HDT) thereof is desired to benot lower than 85° C., preferably in the range of 100 to 140° C.

[1187] The eighth propylene polymer composition may contain, ifnecessary, additives which may be added to the first propylene polymercomposition, with the proviso that the object of the invention is notmarred.

[1188] This propylene polymer composition can be prepared by knownprocesses. For example, the composition can be prepared in accordancewith the processes (1) to (5) described for the first propylene polymercomposition, using the propylene homopolymer (A5) and the olefin polymer(E)

[1189] Such propylene polymer composition is excellent in heatresistance, rigidity and tensile elongation at break.

The Ninth Propylene Polymer Composition

[1190] The ninth propylene polymer composition of the inventioncomprises:

[1191] (A5) a propylene homopolymer which is obtained by polymerizingpropylene in the presence of an olefin polymerization catalystcomprising:

[1192] (i) (h) a transition metal compound represented by the aforesaidformula (I), and

[1193] (ii) at least one compound selected from the group consisting of

[1194] (b) an organoaluminum oxy-compound, and

[1195] (i) a compound which reacts with the transition metal compound(h) to form an ion pair;

[1196] (A6) a propylene polymer which contains constituent units derivedfrom propylene in an amount of not less than 90% by mol and is differentfrom the propylene homopolymer (A5); and

[1197] (D) an olefin elastomer which is characterized in that:

[1198] (1) the elastomer is obtained by polymerizing or copolymerizingat least one monomer selected from olefins of 2 to 20 carbon atoms andpolyenes of 5 to 20 carbon atoms,

[1199] (2) the elastomer contains constituent units derived fromethylene, propylene, butene or 4-methyl-1-pentene in an amount of lessthan 90% by mol, and

[1200] (3) the elastomer has a glass transition temperature (Tg) of nothigher than 10° C.

[1201] Propylene Homopolymer (A5)

[1202] The propylene homopolymer (A5) for constituting the ninthpropylene polymer composition is identical with the propylenehomopolymer (A5) for constituting the sixth propylene polymercomposition.

[1203] Propylene Polymer (A6)

[1204] The propylene polymer (A6) for constituting the ninth propylenepolymer composition is identical with the propylene polymer (A6) forconstituting the sixth propylene polymer composition.

[1205] Olefin Elastomer (D)

[1206] The olefin elastomer (D) for constituting the ninth propylenepolymer composition is identical with the olefin elastomer (D) forconstituting the seventh propylene polymer composition.

[1207] The olefin elastomer can be used in combination of two or morekinds.

[1208] Propylene Polymer Composition

[1209] The ninth propylene polymer composition contains, as itsessential components, the propylene homopolymer (A5), the propylenepolymer (A6) which is different from the propylene homopolymer (A5).,and the olefin elastomer (D). This composition contains the propylenehomopolymer (A5) in an amount of 5 to 95% by weight, the propylenepolymer (A6) in an amount of not more than 95% by weight and the olefinelastomer (D) in an amount of not more than 95% by weight.

[1210] In the ninth propylene polymer composition, it is desired thatthe propylene homopolymer (A5) is contained in an amount of 5 to 95% byweight, preferably 30 to 85% by weight, more preferably 30 to 60% byweight; the propylene polymer (A6) is contained in an amount of 3 to 93%by weight, preferably 5 to 60% by weight, more preferably 30 to 60% byweight; and the olefin elastomer (D) is contained in an amount of 2 to92% by weight, preferably 10 to 65% by weight, more preferably 10 to 40%by weight.

[1211] In the ninth propylene polymer composition, when the intrinsicviscosity ([η]_(A5)) of the propylene homopolymer (A5) and the intrinsicviscosity ([η]_(A6)) of the propylene polymer (A6) has a relation of[η]_(A5)≧[η]_(A6), it is desired that [η]_(A5) is in the range of 1 to10 dl/g, preferably 2 to 5 dl/g; [η]_(A6) is in the range of 0.2 to 1.5dl/g, preferably 0.3 to 1.0 dl/g; and ([η]_(A5)/[η]_(A6)) is in therange of 3 to 30, preferably 4 to 20.

[1212] When the intrinsic viscosity ([η]_(A5)) of the propylenehomopolymer (A5) and the intrinsic viscosity ([η]_(A6)) of the propylenepolymer (A6) has a relation of [η]_(A5)<[η]_(A6), it is desired that[η]_(A5) is in the range of 0.2 to 1.5 dl/g, preferably 0.3 to 1.0 dl/g;[η]_(A6) is in the range of 1 to 10 dl/g, preferably 2 to 5 dl/g; and([η]_(A6)/[η]_(A5)) is in the range of 3 to 30, preferably 4 to 20.

[1213] The ninth propylene polymer composition is desired to have MFR,as measured at 230° C. under a load of 2.16 kg, of 0.01 to 1,000 g/10min, preferably 0.5 to 200 g/10 min. In this composition, Mw/Mn of allthe propylene components for constituting the composition is desirablyin the range of 4 to 15.

[1214] The density of the ninth propylene polymer composition is desiredto be in the range of 0.88 to 0.92 g/cm³, preferably 0.90 to 0.92 g/cm³.

[1215] The flexural modulus (FM) thereof is desired to be in the rangeof 8,000 to 21,000 kg/cm², preferably 12,000 to 20,000 kg/cm².

[1216] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 10 to 60 kg·cm/cm, preferably 15 to 60 kg·cm/cm.

[1217] The tensile elongation at break (EL) thereof is desired to be inthe range of 200 to 1,000%, preferably 300 to 1,000%.

[1218] The heat distortion temperature (HDT) thereof is desired to benot lower than 85° C., preferably in the range of 95 to 140° C.

[1219] The ninth propylene polymer composition may contain, ifnecessary, additives which may be added to the first propylene polymercomposition, with the proviso that the object of the invention is notmarred.

[1220] The ninth propylene polymer composition can be prepared by knownprocesses. For example, the composition can be prepared in accordancewith the processes (1) to (5) described for the first propylene polymercomposition, using the propylene homopolymer (A5), the propylene polymer(A6) and the olefin elastomer (D).

[1221] Such ninth propylene polymer composition is excellent in not onlyheat resistance, rigidity and tensile elongation at break but alsomoldability and impact resistance.

[1222] The ninth propylene polymer composition can be favorably used forvarious structural materials such as those of automobiles and electricalappliances, daily necessaries, various films and sheets.

The Tenth Propylene Polymer Composition

[1223] The tenth propylene polymer composition of the inventioncomprises:

[1224] (A5) a propylene homopolymer which is obtained by polymerizingpropylene in the presence of an olefin polymerization catalystcomprising:

[1225] (i) (h) a transition metal compound represented by the aforesaidformula (I), and

[1226] (ii) at least one compound selected from the group consisting of

[1227] (b) an organoaluminum oxy-compound, and

[1228] (i) a compound which reacts with the transition metal compound(h) to form an ion pair;

[1229] (A6) a propylene polymer which contains constituent units derivedfrom propylene in an amount of not less than 90% by mol and is differentfrom the propylene homopolymer (A5); and

[1230] (E) an olefin polymer which contains constituent units derivedfrom one monomer selected from the group consisting of ethylene, buteneand 4-methyl-1-pentene in an amount of not less than 90% by mol.

[1231] Propylene Homopolymer (A5)

[1232] The propylene homopolymer (A5) for constituting the tenthpropylene polymer composition is identical with the propylenehomopolymer (A5) for constituting the sixth propylene polymercomposition.

[1233] Propylene Polymer (A6)

[1234] The propylene polymer (A6) for constituting the tenth propylenepolymer composition is identical with the propylene polymer (A6) forconstituting the sixth propylene polymer composition.

[1235] Olefin Polymer (E)

[1236] The olefin polymer (E) for constituting the tenth propylenepolymer composition is identical with the olefin polymer (E) forconstituting the eighth propylene polymer composition.

[1237] The olefin polymer (E) can be used in combination of two or morekinds.

[1238] Propylene Polymer Composition

[1239] The tenth propylene polymer composition contains, as itsessential components, the propylene homopolymer (A5), the propylenepolymer (A6) which is different from the propylene homopolymer (AS), andthe olefin polymer (E). This composition contains the propylenehomopolymer (AS) in an amount of 5 to 95% by weight, the propylenepolymer (A6) in an amount of not more than 95% by weight and the olefinpolymer (E) in an amount of not more than 95% by weight.

[1240] In the tenth propylene polymer composition, it is desired thatthe propylene homopolymer (AS) is contained in an amount of 5 to 95% byweight, preferably 30 to 85% by weight, more preferably 30 to 60% byweight; the propylene polymer (A6) is contained in an amount of 3 to 93%by weight, preferably 5 to 60% by weight, more preferably 30 to 60% byweight; and the olefin polymer (E) is contained in an amount of 2 to 92%by weight, preferably 10 to 65% by weight, more preferably 10 to 40% byweight.

[1241] In the tenth propylene polymer composition, when the intrinsicviscosity ([η]_(A5)) of the propylene homopolymer (A5) and the intrinsicviscosity ([η]_(A6)) of the propylene polymer (A6) has a relation of[η]_(A5)≧[η]_(A6), it is desired that [η]_(A5) is in the range of 1 to10 dl/g, preferably 2 to 5 dl/g; [η]_(A6) is in the range of 0.2 to 1.5dl/g, preferably 0.3 to 1.0 dl/g; and ([η]_(A5)/[η]_(A6)) is in therange of 3 to 30, preferably 4 to 20.

[1242] When the intrinsic viscosity ([η]_(A5)) of the propylenehomopolymer (A5) and the intrinsic viscosity ([η]_(A6)) of the propylenepolymer (A6) has a relation of ([η]_(A5)<[η]_(A6)′ it is desired that[η]_(A5) is in the range of 0.2 to 1.5 dl/g, preferably 0.3 to 1.0 dl/g;[η]_(A6) is in the range of 1 to 10 dl/g, preferably 2 to 5 dl/g; and([η]_(A6)/[η]_(A5)) is in the range of 3 to 30, preferably 4 to 20.

[1243] The tenth propylene polymer composition is desired to have MFR,as measured at 230° C. under a load of 2.16 kg, of 0.01 to 1,000 g/10min, preferably 0.5 to 200 g/10 min. In this composition, Mw/Mn of allthe propylene components for constituting the composition is desirablyin the range of 4 to 15.

[1244] The density of the tenth propylene polymer composition is desiredto be in the range of 0.80 to 0.98 g/cm³, preferably 0.85 to 0.94 g/cm³.

[1245] The flexural modulus (FM) thereof is desired to be in the rangeof 12,000 to 21,000 kg/cm², preferably 14,000 to 20,000 kg/cm².

[1246] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 2 to 20 kg·cm/cm, preferably 2 to 10 kg·cm/cm.

[1247] The tensile elongation at break (EL) thereof is desired to be inthe range of 100 to 500%, preferably 200 to 400%.

[1248] The heat distortion temperature (HDT) thereof is desired to benot lower than 85° C., preferably in the range of 100 to 140° C.

[1249] The tenth propylene polymer composition may contain, ifnecessary, additives which may be added to the first propylene polymercomposition, with the proviso that the object of the invention is notmarred.

[1250] The tenth propylene polymer composition can be prepared by knownprocesses. For example, the composition can be prepared in accordancewith the processes (1) to (5) described for the first propylene polymercomposition, using the propylene homopolymer (A5), the propylene polymer(A6) and the olefin polymer (E).

[1251] Such tenth propylene polymer composition is excellent in not onlyheat resistance, rigidity and tensile elongation at break but alsomoldability.

The Eleventh Propylene Polymer Composition

[1252] The eleventh propylene polymer composition of the inventioncomprises:

[1253] (A5) a propylene homopolymer which is obtained by polymerizingpropylene in the presence of an olefin polymerization catalystcomprising:

[1254] (i) (h) a transition metal compound represented by the aforesaidformula (I), and

[1255] (ii) at least one compound selected from the group consisting of

[1256] (b) an organoaluminum oxy-compound, and

[1257] (i) a compound which reacts with the transition metal compound(h) to form an ion pair;

[1258] (D) an olefin elastomer which is characterized in that:

[1259] (1) the elastomer is obtained by polymerizing or copolymerizingat least one monomer selected from olefins of 2 to 20 carbon atoms andpolyenes of 5 to 20 carbon atoms,

[1260] (2) the elastomer contains constituent units derived fromethylene, propylene, butene or 4-methyl-1-pentene in an amount of lessthan 90% by mol, and

[1261] (3) the elastomer has a glass transition temperature (Tg) of nothigher than 10° C.; and

[1262] (E) an olefin polymer which contains constituent units derivedfrom one monomer selected from the group consisting of ethylene, buteneand 4-methyl-1-pentene in an amount of not less than 90% by mol.

[1263] Propylene Homopolymer (A5)

[1264] The propylene homopolymer (A5) for constituting the eleventhpropylene polymer composition is identical with the propylenehomopolymer (A5) for constituting the sixth propylene polymercomposition.

[1265] Olefin Elastomer (D)

[1266] The olefin elastomer (D) for constituting the eleventh propylenepolymer composition is identical with the olefin elastomer (D) forconstituting the seventh propylene polymer composition.

[1267] The olefin polymer (D) can be used in combination of two or morekinds.

[1268] Olefin Polymer (E)

[1269] The olefin polymer (E) for constituting the eleventh propylenepolymer composition is identical with the olefin polymer (E) forconstituting the eighth propylene polymer composition.

[1270] The olefin polymer (E) can be used in combination of two or morekinds.

[1271] Propylene Polymer Composition

[1272] The eleventh propylene polymer composition contains, as itsessential components, the propylene homopolymer (A5), the olefinelastomer (D) and the olefin polymer (E). This composition contains thepropylene homopolymer (A5) in an amount of 5 to 95% by weight, theolefin elastomer (D) in an amount of not more than 95% by weight and theolefin polymer (E) in an amount of not more than 95% by weight.

[1273] In the eleventh propylene polymer composition, it is desired thatthe propylene homopolymer (A5) is contained in an amount of 5 to 95% byweight, preferably 30 to 85% by weight, more preferably 50 to 70% byweight; the olefin elastomer (D) is contained in an amount of 3 to 93%by weight, preferably 10 to 65% by weight, more preferably 20 to 40% byweight; and the olefin polymer (E) is contained in an amount of 2 to 92%by weight, preferably 5 to 60% by weight, more preferably 10 to 30% byweight.

[1274] The eleventh propylene polymer composition is desired to haveMFR, as measured at 230° C. under a load of 2.16 kg, of 0.01 to 1,000g/10 min, preferably 0.5 to 200 g/10 min. In this composition, Mw/Mn ofall the propylene components for constituting the composition isdesirably in the range of 1.5 to 3.5.

[1275] The density of the eleventh propylene polymer composition isdesired to be in the range of 0.88 to 0.93 g/cm³, preferably 0.90 to0.93 g/cm³.

[1276] The flexural modulus (FM) thereof is desired to be in the rangeof 8,000 to 21,000 kg/cm², preferably 12,000 to 20,000 kg/cm².

[1277] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 10 to 60 kg·cm/cm, preferably 20 to 60 kg·cm/cm.

[1278] The tensile elongation at break (EL) thereof is desired to be inthe range of 200 to 1,000%, preferably 300 to 1,000%.

[1279] The heat distortion temperature (HDT) thereof is desired to benot lower than 85° C., preferably in the range of 95 to 140° C.

[1280] The eleventh propylene polymer composition may contain, ifnecessary, additives which may be added to the first propylene polymercomposition, with the proviso that the object of the invention is notmarred.

[1281] The eleventh propylene polymer composition can be prepared byknown processes. For example, the composition can be prepared inaccordance with the processes (1) to (5) described for the firstpropylene polymer composition, using the propylene homopolymer (AS), theolefin elastomer (D) and the olefin polymer (E).

[1282] Such eleventh propylene polymer composition is excellent in notonly heat resistance, rigidity and tensile elongation at break but alsoimpact resistance.

[1283] The eleventh propylene polymer composition can be favorably usedfor various structural materials such as those of automobiles andelectrical appliances, daily necessaries, various films and sheets.

The Twelfth Propylene Polymer Composition

[1284] The twelfth propylene polymer composition of the inventioncomprises:

[1285] (A5) a propylene homopolymer which is obtained by polymerizingpropylene in the presence of an olefin polymerization catalystcomprising:

[1286] (i) (h) a transition metal compound represented by the aforesaidformula (I), and

[1287] (ii) at least one compound selected from the group consisting of

[1288] (b) an organoaluminum oxy-compound, and

[1289] (i) a compound which reacts with the transition metal compound(h) to form an ion pair;

[1290] (A6) a propylene polymer which contains constituent units derivedfrom propylene in an amount of not less than 90% by mol and is differentfrom the propylene homopolymer (AS);

[1291] (D) an olefin elastomer which is characterized in that:

[1292] (1) the elastomer is obtained by polymerizing or copolymerizingat least one monomer selected from olefins of 2 to 20 carbon atoms andpolyenes of 5 to 20 carbon atoms,

[1293] (2) the elastomer contains constituent units derived fromethylene, propylene, butene or 4-methyl-1-pentene in an amount of lessthan 90% by mol, and

[1294] (3) the elastomer has a glass transition temperature (Tg) of nothigher than 10° C.; and

[1295] (E) an olefin polymer which contains constituent units derivedfrom one monomer selected from the group consisting of ethylene, buteneand 4-methyl-1-pentene in an amount of not less than 90% by mol.

[1296] Propylene Homopolymer (A5)

[1297] The propylene homopolymer (A5) for constituting the twelfthpropylene polymer composition is identical with the propylenehomopolymer (A5) for constituting the sixth propylene polymercomposition. Propylene polymer (A6)

[1298] The propylene polymer (A6) for constituting the twelfth propylenepolymer composition is identical with the propylene polymer (A6) forconstituting the sixth propylene polymer composition.

[1299] Olefin Elastomer (D)

[1300] The olefin elastomer (D) for constituting the twelfth propylenepolymer composition is identical with the olefin elastomer (D) forconstituting the seventh propylene polymer composition.

[1301] The olefin elastomer (D) can be used in combination of two ormore kinds.

[1302] Olefin Polymer (E)

[1303] The olefin polymer (E) for constituting the twelfth propylenepolymer composition is identical with the olefin polymer (E) forconstituting the eighth propylene polymer composition.

[1304] The olefin polymer (E) can be used in combination of two or morekinds.

[1305] Propylene Polymer Composition

[1306] The twelfth propylene polymer composition contains, as itsessential components, the propylene homopolymer (A5), the propylenepolymer (A6) which is different from the propylene homopolymer (A5), theolefin elastomer (D) and the olefin polymer (E). This compositioncontains the propylene homopolymer (A5) in an amount of 5 to 95% byweight, the propylene polymer (A6) in an amount of not more than 95% byweight, the olefin elastomer (D) in an amount of not more than 95% byweight and the olefin polymer (E) in an amount of not more than 95% byweight.

[1307] In the twelfth propylene polymer composition, it is desired thatthe propylene homopolymer (A5) is contained in an amount of 5 to 95% byweight, preferably 30 to 85% by weight, more preferably 30 to 50% byweight; the propylene polymer (A6) is contained in an amount of 2 to 92%by weight, preferably 5 to 60% by weight, more preferably 30 to 50% byweight; the olefin elastomer (D) is contained in an amount of 2 to 92%by weight, preferably 5 to 60% by weight, more preferably 10 to 30% byweight; and the olefin polymer (E) is contained in an amount of 1 to 91%by weight, preferably 5 to 60.% by weight, more preferably 10 to 30% byweight.

[1308] In the twelfth propylene polymer composition, when the intrinsicviscosity ([η]_(A5)) of the propylene homopolymer (A5) and the intrinsicviscosity ([η]_(A6)) of the propylene polymer (A6) has a relation of[η]_(A5)≧[η]_(A6), it is desired that [η]_(A5) is in the range of 1 to10 dl/g, preferably 2 to 5 dl/g; [η]_(A6) is in the range of 0.2 to1.5/g, preferably 0.3 to 1.0 dl/g; and ([η]_(A5)/[η]_(A6)) is in therange of 3 to 30, preferably 4 to 20.

[1309] When the intrinsic viscosity ([η]_(A5)) of the propylenehomopolymer (A5) and the intrinsic viscosity ([η]_(A6)) of the propylenepolymer (A6) has a relation of [η]_(A5)<[η]_(A6), it is desired that[η]_(A5) is in the range of 0.2 to 1.5 dl/g, preferably 0.3 to 1.0 dl/g;[η]_(A6) is in the range of 1 to 10 dl/g, preferably 2 to 5 dl/g; and([η]_(A6)/[η]_(A5)) is in the range of 3 to 30, preferably 4 to 20.

[1310] The twelfth propylene polymer composition is desired to have MFR,as measured at 230° C. under a load of 2.16 kg, of 0.01 to 1,000 g/10min, preferably 0.5 to 200 g/10 min.

[1311] In this composition, Mw/Mn of all the propylene components forconstituting the composition is desirably in the range of 4 to 15.

[1312] The density of the twelfth propylene polymer composition isdesired to be in the range of 0.88 to 0.93 g/cm³, preferably 0.90 to0.93 g/cm³.

[1313] The flexural modulus (FM) thereof is desired to be in the rangeof 8,000 to 21,000 kg/cm², preferably 12,000 to 20,000 kg/cm².

[1314] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 10 to 60 kg·cm/cm, preferably 20 to 60 kg·cm/cm.

[1315] The tensile elongation at break (EL) thereof is desired to be inthe range of 200 to 1,000%, preferably 300 to 1,000%.

[1316] The heat distortion temperature (HDT) thereof is desired to benot lower than 85° C., preferably in the range of 95 to 140° C.

[1317] The twelfth propylene polymer composition may contain, ifnecessary, additives which may be added to the first propylene polymercomposition, with the proviso that the object of the invention-is notmarred.

[1318] The twelfth propylene polymer composition can be prepared byknown processes. For example, the composition can be prepared inaccordance with the processes (1) to (5) described for the firstpropylene polymer composition, using the propylene homopolymer (A5), thepropylene polymer (A6), the olefin elastomer (D) and the olefin polymer(E).

[1319] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but alsomoldability and impact resistance.

[1320] The twelfth propylene polymer composition can be favorably usedfor various structural materials such as those of automobiles andelectrical appliances, daily necessaries, various films and sheets.

The Thirteenth Propylene Polymer Composition

[1321] The thirteenth propylene polymer composition comprises:

[1322] (A7) a propylene copolymer which is characterized in that:

[1323] the propylene copolymer is obtained by copolymerizing propyleneand at least one α-olefin selected from ethylene and α-olefins of 4 to20 carbon atoms in the presence of an olefin polymerization catalystcomprising:

[1324] (i) (h) a transition metal compound represented by the aforesaidformula (I), and

[1325] (ii) at least one compound selected from the group consisting of

[1326] (b) an organoaluminum oxy-compound, and

[1327] (i) a compound which reacts with the transition metal compound(h) to form an ion pair, and

[1328] the propylene copolymer contains constituent units derived frompropylene in an amount of not less than 90% by mol; and

[1329] (A6) a propylene polymer which contains constituent units derivedfrom propylene in an amount of not less than 90% by mol and is differentfrom the propylene copolymer (A7).

[1330] Propylene Copolymer (A7)

[1331] The propylene copolymer (A7) is α-random copolymer of propyleneand at least one α-olefin selected from the group consisting of ethyleneand α-olefins of 4 to 20 carbon atoms, which is prepared by the use ofthe olefin polymerization catalyst (4) used for preparation of thepropylene homopolymer (A5).

[1332] In the propylene copolymer (A7), the propylene units arecontained in an amount of not less than 90% by mol, preferably 90 to 98%by mol, more preferably 90 to 96%; and the comonomer units derived froman α-olefin selected from ethylene and α-olefins of 4 to 20 carbon atomsin an amount of not more than 10% by mol, preferably 2 to 10% by mol,more preferably 4 to 10% by mol.

[1333] Examples of the α-olefins of 4 to 20 carbon atoms include1-butene, 0.1-pentene, 1-hexene, 4-methyl-1-pentene, 1-heptene,1-octene, 2-ethyl-1-hexene, 1-decene, 1-dodecene, 1-tetradecene and1-eicosene.

[1334] Preferably used as the comonomers for the copolymerization areethylene, 1-butene, 1-pentene, 1-hexene, 1-octene and 1-decene.

[1335] The propylene copolymer (A7) is desired to have MFR, as measuredat 230° C. under a load of 2.16 kg, of 0.01 to 1,000 g/10 min,preferably 0.5 to 200 g/10 min, and Mw/Mn, as measured by GPC, of 1.5 to3.5, preferably 2.0 to 3.0, more preferably 2.0 to 2.5.

[1336] Further, the propylene copolymer (A7) is desired to have anintrinsic viscosity [η]of 0.1 to 20 dl/g, preferably 0.5 to 10 dl/g,more preferably 1 to 5 dl/g, and a weight-average molecular weight of1×10³ to 500×10⁴, preferably 1×10⁴ to 100×10⁴.

[1337] The crystallinity of the propylene copolymer (A7), as measured byX-ray diffractometry, is desired to be not less than 20%, preferably notless than 30%.

[1338] The triad tacticity (mm fraction) of the propylene copolymer (A7)is desired to be not less than 98.0%, preferably not less than 98.2%,more preferably not less than 98.5%.

[1339] The proportion of the irregularly positioned units based on the2,1-insertion of the propylene monomer is desired to be not more than0.5%, preferably not more than 0.18%, more preferably not more than0.15%.

[1340] The proportion of the irregularly positioned units based-on the1,3-insertion of the propylene monomer is desired to be less than thedetected lower limit by the ¹³C-NMR measurement (less than 0.03%)

[1341] Propylene Polymer (A6)

[1342] The propylene polymer (A6) for constituting the thirteenthpropylene polymer composition is identical with the propylene polymer(A6) for constituting the sixth propylene polymer composition.

[1343] Propylene Polymer Composition

[1344] The thirteenth propylene polymer composition comprises thepropylene copolymer (A7) and the propylene polymer (A6) which isdifferent from the propylene copolymer (A7). In the composition, it isdesired that the propylene copolymer (A7) is contained in an amount of 5to 95% by weight, preferably 15 to 85% by weight, more preferably 30 to70% by weight; and the propylene polymer (A6) is contained in an amountof 5 to 95% by weight, preferably 15 to 85% by weight, more preferably30 to 70% by weight.

[1345] In the thirteenth propylene polymer composition, when theintrinsic viscosity ([η]A7) of the propylene copolymer (A7) and theintrinsic viscosity [η]_(A6)) of the propylene polymer (A6) has arelation of [η]_(A7)≧[η]_(A6), it is desired that [η]_(A7) is in therange of 1 to 10 dl/g, preferably 2 to 0.5 dl/g; [η]_(A6) is in therange of 0.2 to 1.5 dl/g, preferably 0.3 to 1.0 dl/g; and([η]_(A7)/[η]_(A6)) is in the range of 3 to 30, preferably 4 to 20.

[1346] When the intrinsic viscosity ([η]_(A7)) Of the propylenehomopolymer (A7) and the intrinsic viscosity ([η]_(A6)) of the propylenepolymer (A6) has a relation of [η]_(A7)<[η]_(A6)′ it is desired that[η]_(A7) is in the range of 0.2 to 1.5 dl/g, preferably 0.3 to 1.0 dl/g;[η]_(A6) is in the range of 1 to 10 dl/g, preferably 2 to 5 dl/g; and[η]_(A6/1)[η]_(A7)) is in the range of 3 to 30, preferably 4 to 20.

[1347] The thirteenth propylene polymer composition is desired to haveMFR, as measured at 230° C. under a load of 2.16 kg, of 0.01 to 1,000g/10 min, preferably 0.5 to 200 g/10 min. In this composition, Mw/Mn ofall the propylene components for constituting the composition isdesirably in the range of 4 to 15.

[1348] The density of the thirteenth propylene polymer composition isdesired to be in the range of 0.88 to 0.92 g/cm³, preferably 0.89 to0.92 g/cm³.

[1349] The flexural modulus (FM) thereof is desired to be in the rangeof 2,000 to 20,000 kg/cm², preferably 4,000 to 15,000 kg/cm².

[1350] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 2 to 20 kg·cm/cm, preferably 5 to 20 kg·cm/cm.

[1351] The tensile elongation at break (EL) thereof is desired to be inthe range of 100 to 2,000. %, preferably 200 to 1,000%.

[1352] The heat distortion temperature (HDT) thereof is 25 desired to benot lower than 80° C., preferably in the range of 90 to 140° C.

[1353] The thirteenth propylene polymer composition may contain, ifnecessary, additives which may be added to the first propylene polymercomposition, with the proviso that the object of the invention is notmarred.

[1354] The thirteenth propylene polymer composition can be prepared byknown processes. For example, the composition can be prepared inaccordance with the processes (1) to (5) described for the firstpropylene polymer composition, using the propylene copolymer (A7) andthe propylene polymer (A6).

[1355] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but alsomoldability.

The Fourteenth Propylene Composition

[1356] The fourteenth propylene polymer composition comprises:

[1357] (A7) a propylene copolymer which is characterized in that:

[1358] the propylene copolymer is obtained by copolymerizing propyleneand at least one α-olefin selected from ethylene and α-olefins of 4 to20 carbon atoms in the presence of an olefin polymerization catalystcomprising:

[1359] (i) (h) a transition metal compound represented by the aforesaidformula (I), and

[1360] (ii) at least one compound selected from the group consisting of

[1361] (b) an organoaluminum oxy-compound, and

[1362] (i) a compound which reacts with the transition metal compound(h) to form an ion pair, and the propylene copolymer containsconstituent units derived from propylene in an amount of not less than90% by mol; and

[1363] (D) an olefin elastomer which is characterized in that:

[1364] (1) the elastomer is obtained by polymerizing or copolymerizingat least one monomer selected from olefins of 2 to 20 carbon atoms andpolyenes of 5 to 20 carbon atoms,

[1365] (2) the elastomer contains constituent units derived fromethylene, propylene, butene or 4-methyl-1-pentene in an amount of lessthan 90% by mol, and

[1366] (3) the elastomer has a glass transition temperature (Tg) of nothigher than 10° C.

[1367] Propylene Copolymer (A7)

[1368] The propylene copolymer (A7) for constituting the fourteenthpropylene polymer composition is identical with the propylene copolymer(A7) for constituting the thirteenth propylene polymer composition.

[1369] Olefin Elastomer (D)

[1370] The olefin elastomer (D) for constituting the fourteenthpropylene polymer composition is identical with the olefin elastomer (D)for constituting the seventh propylene polymer composition.

[1371] The olefin elastomer (D) can be used in combination of two ormore kinds.

[1372] Propylene Polymer Composition.

[1373] The fourteenth propylene polymer composition comprises thepropylene copolymer (A7) and the olefin elastomer (D).

[1374] In this composition, it is desired that the propylene copolymer(A7) is contained in an amount of 5 to 95% by weight, preferably 30 to90% by weight, more preferably 50 to 80% by weight; and the olefinelastomer (D) is contained in an amount of 5 to 95% by weight,preferably 10 to 70% by weight, more preferably 20 to 50% by weight.

[1375] The fourteenth propylene polymer composition is desired to haveMFR, as measured at 230° C. under a load of 2.16 kg, of 0.01 to 1,000g/10 min, preferably 0.5 to 200 g/10 min. In this composition, Mw/Mn ofall the propylene components for constituting the composition isdesirably in the range of 1.5 to 3.5.

[1376] The density of the fourteenth propylene polymer composition isdesired to be in the range of 0.87 to 0.92 g/cm³; preferably 0.88 to0.92 g/cm³.

[1377] The flexural modulus (FM) thereof is desired to be in the rangeof 2,000 to 20,000 kg/cm², preferably 4,000 to 15,000 kg/cm².

[1378] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 10 to 60 kg·cm/cm, preferably 20 to 60 kg·cm/cm.

[1379] The tensile elongation at break (EL) thereof is desired to be inthe range of 200 to 2,000%, preferably 200 to 1,000%.

[1380] The heat distortion temperature (HDT) thereof is desired to benot lower than 80° C., preferably in the range of 90 to 140° C.

[1381] The fourteenth propylene polymer composition may contain, ifnecessary, additives which may be added to the first propylene polymercomposition, with the proviso that the object of the invention is notmarred.

[1382] This propylene polymer composition can be prepared by knownprocesses. For example, the composition can be prepared in accordancewith the processes (1) to (5) described for the, first propylene polymercomposition, using the propylene copolymer (A7) and the olefin elastomer

[1383] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but also impactresistance.

[1384] The fourteenth propylene polymer composition can be favorablyused-for various structural materials such as those of automobiles andelectrical appliances, daily necessaries and various sheets.

The Fifteenth Propylene Polymer Composition

[1385] The fifteenth propylene polymer composition of the inventioncomprises:

[1386] (A7) a propylene copolymer which is characterized in that:

[1387] the propylene copolymer is obtained by copolymerizing propyleneand at least one α-olefin selected from ethylene and α-olefins of 4 to20 carbon atoms in the presence of an olefin polymerization catalystcomprising:

[1388] (i) (h) a transition metal compound represented by the aforesaidformula (I), and

[1389] (ii) at least one compound selected from the group consisting of

[1390] (b) an organoaluminum oxy-compound, and

[1391] (i) a compound which reacts with the transition metal compound(h) to-form an ion pair, and the propylene copolymer containsconstituent units derived from propylene in an amount of not less than90% by mol; and

[1392] (E) an olefin polymer which contains constituent units derivedfrom one monomer selected from the group consisting of ethylene, buteneand 4-methyl-1-pentene in an amount of not less than 90% by mol.

[1393] Propylene Copolymer (A7)

[1394] The propylene copolymer (A7) for constituting the fifteenthpropylene polymer composition is identical with the propylene copolymer(A7) for constituting the thirteenth propylene polymer composition.

[1395] Olefin Polymer (E)

[1396] The olefin polymer (E) for constituting the fifteenth propylenepolymer composition is identical with the olefin polymer (E) forconstituting the eighth propylene polymer composition.

[1397] The olefin polymer (E) can be used in combination of two or morekinds.

[1398] Propylene polymer composition

[1399] The fifteenth propylene polymer composition comprises thepropylene copolymer (A7) and the olefin polymer (E). In thiscomposition, it is desired that the propylene copolymer (A7) iscontained in an amount of 5 to 95% by weight, preferably 30 to 90% byweight, more preferably 50 to 80% by weight; and the olefin polymer (E)is contained in an amount of 5 to 95% by weight, preferably 10 to 70% byweight, more preferably 20 to 50% by weight.

[1400] The fifteenth propylene polymer composition is desired to haveMFR, as measured at 230° C. under a load of 2.16 kg, of 0.1 to 1,000g/10 min, preferably 0.5 to 200 g/10 min. In this composition, Mw/Mn ofall the propylene components for constituting the composition isdesirably in the range of 1.5 to 3.5.

[1401] The density of the fifteenth propylene polymer composition isdesired to be in the range of 0.80 to 0.98 g/cm³, preferably 0.85 to0.94 g/cm³.

[1402] The flexural modulus (FM) thereof is desired to be in the rangeof 2,000 to 20,000 kg/cm², preferably 4,000 to 15,000 kg/cm².

[1403] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 2 to 20 kg·cm/cm, preferably 5 to 20 kg·cm/cm.

[1404] The tensile elongation at break (EL) thereof is desired to be inthe range of 100 to 2,000%, preferably 200 to 1,000%.

[1405] The heat distortion temperature (HDT) thereof is desired to benot lower than 80° C., preferably in the range of 90 to 140° C.

[1406] The fifteenth propylene polymer composition may contain, ifnecessary, additives which may be added to the first propylene polymercomposition, with the proviso that the object of the invention is notmarred.

[1407] This propylene polymer composition can be prepared by knownprocesses. For example, the composition can be prepared in accordancewith the processes (1) to (5) described for the first propylene polymercomposition, using the propylene copolymer (A7) and the olefin polymer(E).

[1408] Such propylene polymer composition is excellent in heatresistance, rigidity and tensile elongation at break.

The Sixteenth Propylene Polymer Composition

[1409] The sixteenth propylene polymer composition of the inventioncomprises:

[1410] (A7) a propylene copolymer which is characterized in that:

[1411] the propylene copolymer is obtained by copolymerizing propyleneand at least one α-olefin selected from ethylene and α-olefins of 4 to20 carbon atoms in the presence of an olefin polymerization catalystcomprising:

[1412] (i) (h) a transition metal compound represented by the aforesaidformula (I), and

[1413] (ii) at least one compound selected from the group consisting of

[1414] (b) an organoaluminum oxy-compound, and

[1415] (i) a compound which reacts with the transition metal compound(h) to form an ion pair, and

[1416] the propylene copolymer contains constituent units derived frompropylene in an amount of not less than 90% by mol;

[1417] (A6) a propylene polymer which contains constituent units derivedfrom propylene in an amount of not less than 90% by mol and is differentfrom the propylene copolymer (A7); and

[1418] (D) an olefin elastomer which is characterized in that:

[1419] (1) the elastomer is obtained by polymerizing or copolymerizingat least one monomer selected from olefins of 2 to 20 carbon atoms andpolyenes of 5 to 20 carbon atoms,

[1420] (2) the elastomer contains constituent units derived fromethylene, propylene, butene or 4-methyl-1-pentene in an amount of lessthan 90% by mol, and

[1421] (3) the elastomer has a glass transition temperature (Tg) of nothigher than 10° C.

[1422] Propylene Copolymer (A7)

[1423] The propylene copolymer (A7) for constituting the sixteenthpropylene polymer composition is identical with the propylene copolymer(A7) for constituting the thirteenth propylene polymer composition.

[1424] Propylene Polymer (A6)

[1425] The propylene polymer (A6) for constituting the sixteenthpropylene polymer composition is identical with the propylene polymer(A6) for constituting the sixth propylene polymer composition.

[1426] Olefin Elastomer (D)

[1427] The olefin elastomer (D) for constituting the sixteenth propylenepolymer composition is identical with the olefin elastomer (D) forconstituting the seventh propylene polymer composition.

[1428] The olefin elastomer (D) can be used in combination of two ormore kinds.

[1429] Propylene Polymer Composition

[1430] The sixteenth propylene polymer composition contains, as itsessential components, the propylene copolymer (A7), the propylenepolymer (A6) which is different from the propylene copolymer (A7), andthe olefin elastomer (D). This composition contains the propylenecopolymer (A7) in an amount of 5 to 95% by weight, the propylene polymer(A6) in an amount of not more than 95% by weight and the olefinelastomer (D) in an amount of not more than 95% by weight.

[1431] In the sixteenth propylene polymer composition, it is desiredthat the propylene copolymer (A7) is contained in an amount of 5 to 95%by weight, preferably 30 to 85% by weight, more preferably 30 to 60% byweight; the propylene polymer (A6) is contained in an amount of 3 to 93%by weight, preferably 5 to 60% by weight, more preferably 30 to 60% byweight; and the olefin elastomer (D) is contained in an amount of 2 to92% by weight, preferably 10 to 65% by weight, more preferably 10 to 40%by weight.

[1432] In the sixteenth propylene polymer composition, when theintrinsic viscosity ([η]_(A7)) of the propylene copolymer (A7) and theintrinsic viscosity ([η]_(A6)) of the propylene polymer (A6) has arelation of [η]_(A7)≧[η]_(A6), it is desired that [η]_(A7) is in therange of 1 to 10 dl/g, preferably 2 to 5 dl/g; [η]_(A6) is in the rangeof 0.2 to 1.5 dl/g, preferably 0.3 to 1.0 dl/g; and ([η]_(A7)/[η]_(A6))is in the range of 3 to 30, preferably 4 to 20.

[1433] When the intrinsic viscosity ([η]_(A7)) of the propylenecopolymer (A7) and the intrinsic viscosity ([η]_(A6)) of the propylenepolymer (A6) has a relation of [η]_(A7)<[η]_(A6), it is desired that[η]_(A7) is in the range of 0.2 to 1.5 dl/g, preferably 0.3 to 1.0 dl/g;[η]_(A6) is in the range of 1 to 10 dl/g, preferably 2 to 5 dl/g; and([η]_(A6)/[η]_(A7)) is in the range of 3 to 30, preferably 4 to 20.

[1434] The sixteenth propylene polymer composition is desired to haveMFR, as measured at 230° C. under a load of 2.16 kg, of 0.01 to 1,000g/10 min, preferably 0.5 to 200 g/10 min. In this composition, Mw/Mn ofall the propylene components for constituting the composition isdesirably in the range of 4 to 15.

[1435] The density of the sixteenth propylene polymer composition isdesired to be in the range of 0.87 to 0.92 g/cm³, preferably 0.88 to0.92 g/cm³.

[1436] The flexural modulus (FM) thereof is desired to be in the rangeof 2,000 to 20,000 kg/cm², preferably 4,000 to 15,000 kg/cm².

[1437] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 10 to 60 kg·cm/cm, preferably 20 to 60 kg·cm/cm.

[1438] The tensile elongation at break (EL) thereof is desired to be inthe range of 200 to 2,000%, preferably 200 to 1,000%.

[1439] The heat distortion temperature (HDT) thereof is desired to benot-lower than 80° C., preferably in the range of 90 to 0.140° C.

[1440] The sixteenth propylene polymer composition may contain, ifnecessary, additives which may be added to the first propylene polymercomposition, with the proviso that the object of the invention is notmarred.

[1441] The sixteenth propylene polymer composition can be prepared byknown processes. For example, the composition can be prepared inaccordance with the processes (1) to (5) described for the firstpropylene polymer composition, using the propylene copolymer (A7), thepropylene polymer (A6) and the olefin elastomer (D).

[1442] Such sixteenth propylene polymer composition is excellent in notonly heat resistance, rigidity and tensile elongation at break but alsomoldability and impact resistance.

[1443] The sixteenth propylene polymer composition can be favorably usedfor various structural materials such as those of automobiles andelectrical appliances, daily necessaries, various films and sheets.

The Seventeenth Propylene Polymer Composition

[1444] The seventeenth propylene polymer composition of the inventioncomprises:

[1445] (A7) a propylene copolymer which is characterized in that:

[1446] the propylene copolymer is obtained by copolymerizing propyleneand at least one α-olefin selected from ethylene and α-olefins of 4 to20 carbon atoms in the presence of an olefin polymerization catalystcomprising:

[1447] (i) (h) a transition metal compound represented by the aforesaidformula (I), and

[1448] (ii) at least one compound selected from the group consisting of

[1449] (b) an organoaluminum oxy-compound, and

[1450] (i) a compound which reacts with the transition metal compound(h) to form an ion pair, and the propylene copolymer containsconstituent units derived from propylene in an amount of not less than90% by mol;

[1451] (A6) a propylene polymer which contains constituent units derivedfrom propylene in an amount of not less than 90% by mol and is differentfrom the propylene copolymer (A7); and

[1452] (E) an olefin polymer which contains constituent units derivedfrom one monomer selected from the group consisting of ethylene, buteneand 4-methyl-1-pentene in an amount of not less than 90% by mol.

[1453] Propylene Copolymer (A7)

[1454] The propylene copolymer (A7) for constituting the seventeenthpropylene polymer composition is identical with the propylene copolymer(A7) for constituting the thirteenth propylene polymer composition.

[1455] Propylene Polymer (A6)

[1456] The propylene polymer (A6) for constituting the seventeenthpropylene polymer composition is identical with the propylene polymer(A6) for constituting the sixth propylene polymer composition.

[1457] Olefin Polymer (E)

[1458] The olefin polymer (E) for constituting the seventeenth propylenepolymer composition is identical with the olefin polymer (E) forconstituting the eighth propylene polymer composition.

[1459] The olefin polymer (E) can be used in combination of two or morekinds.

[1460] Propylene Polymer Composition

[1461] The seventeenth propylene polymer composition contains, as itsessential components, the propylene copolymer (A7), the propylenepolymer (A6) which is different from the propylene copolymer (A7), andthe olefin polymer (E). This composition contains the propylenecopolymer (A7) in an amount of 5 to 95% by weight, the propylene polymer(A6) in an amount of not more than 95% by weight and the olefin polymer(E) in an amount of not more than 95% by weight.

[1462] In the seventeenth propylene polymer composition, it is desiredthat the propylene copolymer (A7) is contained in an amount of 5 to 95%by weight, preferably 30 to 85% by weight, more preferably 30 to 60% byweight; the propylene polymer (A6) is contained in an amount of 3 to 93%by weight, preferably 5 to 60% by weight, more preferably 30 to 60% byweight; and the olefin polymer (E) is contained in an amount of 2 to 92%by weight, preferably 10 to 65% by weight, more preferably 10 to 40% byweight.

[1463] In the seventeenth propylene polymer composition, when theintrinsic viscosity ([η_(A7)]) of the propylene copolymer (A7) and theintrinsic viscosity ([η]_(A6)) of the propylene polymer (A6) has arelation of [η]_(A7)≧[η]_(A)6, it is desired that [η]_(A7) is in therange of 1 to 10 dl/g, preferably 2 to 5 dl/g; [η]_(A6) is in the rangeof 0.2 to 1.5 dl/g, preferably 0.3 to 1.0 dl/g; and ([η]_(A7/[η]) _(A6))is in the range of 3 to 30, preferably 4 to 20.

[1464] When the intrinsic viscosity ([η]_(A7)) of the propylenecopolymer (A7) and the intrinsic viscosity ([η]_(A6)) of the propylenepolymer (A6) has a relation of [η]_(A7)<[η]_(A6), it is desired that[η]_(A7) is in the range of 0.2 to 1.5 dl/g, preferably 0.3 to 1.0 dl/g;[η]_(A6) is in the range of 1 to 10 dl/g, preferably 2 to 5 dl/g; and([η]_(A6)/[η]_(A7)) is in the range of 3 to 30, preferably to 20.

[1465] The seventeenth propylene polymer composition is desired to haveMFR, as measured at 230° C. under a load of 2.16 kg, of 0.01 to 1,000g/10 min, preferably 0.5 to 200 g/10 min. In this composition, Mw/Mn ofall the propylene components for constituting the composition isdesirably in the range of 4 to 15.

[1466] The density of the seventeenth propylene polymer composition isdesired to be in the range of 0.80 to 0.98 g/cm³, preferably 0.85 to0.94 g/cm³.

[1467] The flexural modulus (FM) thereof is desired to be in the rangeof 2,000 to 20,000 kg/cm², preferably 4,000 to 15,000 kg/cm².

[1468] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 2 to 20 kg·cm/cm, preferably 5 to 20 kg·cm/cm.

[1469] The tensile elongation at break (EL) thereof is desired to be inthe range of 100 to 2,000%, preferably 200 to 1,000%.

[1470] The heat distortion temperature (HDT) thereof is desired to benot lower than 80° C., preferably in the range of 90 to 140° C.

[1471] The seventeenth propylene polymer composition may contain, ifnecessary, additives which may be added to the first propylene polymercomposition, with the proviso that the object of the invention is notmarred.

[1472] The seventeenth propylene polymer composition can be prepared byknown processes. For example, the composition can be prepared inaccordance with the processes (1) to (5) described for the firstpropylene polymer composition, using the propylene copolymer (A7), thepropylene polymer (A6) and the olefin polymer (E).

[1473] Such seventeenth propylene polymer composition is excellent innot only heat resistance, rigidity and tensile elongation at break butalso moldability.

The Eighteenth Propylene Polymer Composition

[1474] The eighteenth propylene polymer composition of the inventioncomprises:

[1475] (A7) a propylene copolymer which is characterized in that:

[1476] the propylene copolymer is obtained by copolymerizing propyleneand at least one α-olefin selected from ethylene and α-olefins of 4 to20 carbon atoms in the presence of an olefin polymerization catalystcomprising:

[1477] (i) (h) a transition metal compound represented by the aforesaidformula (I), and

[1478] (ii) at least one compound selected from the group consisting of

[1479] (b) an organoaluminum oxy-compound, and

[1480] (i) a compound which reacts with the transition metal compound(h) to form an ion pair, and

[1481] the propylene copolymer contains constituent units derived frompropylene in an amount of not less than 90% by mol;

[1482] (D) an olefin elastomer which is characterized in that:

[1483] (1) the elastomer is obtained by polymerizing or copolymerizingat least one monomer selected from olefins of 2 to 20 carbon atoms andpolyenes of 5 to 20 carbon atoms,

[1484] (2) the elastomer contains constituent units derived fromethylene, propylene, butene or 4-methyl-1-pentene in an amount of lessthan 90% by mol, and

[1485] (3) the elastomer has a glass transition temperature (Tg) of nothigher than 10° C.; and

[1486] (E) an olefin polymer which contains constituent units derivedfrom one monomer selected from the group consisting of ethylene, buteneand 4-methyl-1-pentene in an amount of not less than 90% by mol.

[1487] Propylene Copolymer (A7)

[1488] The propylene copolymer (A7) for constituting the eighteenthpropylene polymer composition is identical with the propylene copolymer(A7) for constituting the thirteenth propylene polymer composition.

[1489] Olefin Elastomer (D)

[1490] The olefin elastomer (D) for constituting the eighteenthpropylene polymer composition is identical with the olefin elastomer (D)for constituting the seventh propylene polymer composition.

[1491] The olefin elastomer (D) can be used in combination of two ormore kinds.

[1492] Olefin Polymer (E)

[1493] The olefin polymer (E) for constituting the eighteenth propylenepolymer composition is identical with the olefin polymer (E) forconstituting the eighth propylene polymer composition.

[1494] The olefin polymer (E) can be used in combination of two or morekinds.

[1495] Propylene Polymer Composition

[1496] The eighteenth propylene polymer composition contains, as itsessential components, the propylene copolymer (A7), the olefin elastomer(D) and the olefin polymer (E). This composition contains the propylenecopolymer (A7) in an amount of 5 to 95% by weight, the olefin elastomer(D) in an amount of not more than 95% by weight and the olefin polymer(E) in an amount of not more than 95% by weight.

[1497] In the eighteenth propylene polymer composition, it is desiredthat the propylene copolymer (A7) is contained in an amount of 5 to 95%by weight, preferably 30 to 85% by weight, more preferably 50 to 70% byweight; the olefin elastomer (D) is contained in an amount of 3 to 93%by weight, preferably 10 to 65% by weight, more preferably 20 to 40% byweight; and the olefin polymer (E) is contained in an amount of 2 to 92%by weight, preferably 5 to 60% by weight, more preferably 10 to 30% byweight.

[1498] The eighteenth propylene polymer composition is desired to haveMFR, as measured at 230° C. under a load of 2.16 kg, of 0.01 to 1,000g/10 min, preferably 0.5 to 200 g/10 min. In this composition, Mw/Mn ofall the propylene components for constituting the composition isdesirably in the range of 1.5 to 3.5.

[1499] The density of the eighteenth propylene polymer composition isdesired to be in the range of 0.87 to 0.92 g/cm³, preferably 0.88 to0.92 g/cm³.

[1500] The flexural modulus (FM) thereof is desired to be in the rangeof 2,000 to 20,000 kg/cm², preferably 4,000 to 15,000 kg/cm².

[1501] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 10 to 60 kg·cm/cm, preferably 20 to 60 kg·cm/cm.

[1502] The tensile elongation at break (EL) thereof is desired to be inthe range of 200 to 2,000%, preferably 200 to 1,000%.

[1503] The heat distortion temperature (HDT) thereof is desired to benot lower than 80° C., preferably in the range of 90 to 140° C.

[1504] The eighteenth propylene polymer composition may contain, ifnecessary, additives which may be added to the first propylene polymercomposition, with the proviso that the object of the invention is notmarred.

[1505] The eighteenth propylene polymer composition can be prepared byknown processes. For example, the composition can be prepared inaccordance with the processes (1) to (5) described for the firstpropylene polymer composition, using the propylene copolymer (A7), theolefin elastomer (D) and the olefin polymer (E).

[1506] Such eighteenth propylene polymer composition is excellent in notonly heat resistance, rigidity and tensile elongation at break but alsoimpact resistance.

[1507] The eighteenth propylene polymer composition can be favorablyused for various structural materials such as those of automobiles andelectrical appliances, daily necessaries, various films and sheets.

The Nineteenth Propylene Polymer Composition

[1508] The nineteenth propylene polymer composition of the inventioncomprises:

[1509] (A7) a propylene copolymer which is characterized in that:

[1510] the propylene copolymer is obtained by copolymerizing propyleneand at least one α-olefin selected from ethylene and α-olefins of 4 to20 carbon atoms in the presence of an olefin polymerization catalystcomprising:

[1511] (i) (h) a transition metal compound represented by the aforesaidformula (I), and

[1512] (ii) at least one compound selected from the group consisting of

[1513] (b) an organoaluminum oxy-compound, and

[1514] (i) a compound which reacts with the transition metal compound(h) to form an ion pair, and the propylene copolymer containsconstituent units derived from propylene in an amount of not less than90% by mol;

[1515] (A6) a propylene polymer which contains constituent units derivedfrom propylene in an amount of not less than 90% by mol and is differentfrom the propylene copolymer (A7);

[1516] (D) an olefin elastomer which is characterized in that:

[1517] (1) the elastomer is obtained by polymerizing or copolymerizingat least one monomer selected from olefins of 2 to 20 carbon atoms andpolyenes of 5 to 20 carbon atoms,

[1518] (2) the elastomer contains constituent units derived fromethylene, propylene, butene or 4-methyl-1-pentene in an amount of lessthan 90% by mol, and

[1519] (3) the elastomer has a glass transition temperature (Tg) of nothigher than 10° C.; and

[1520] (E) an olefin polymer which contains constituent units derivedfrom one monomer selected from the group consisting of ethylene, buteneand 4-methyl-1-pentene in an amount of not less than 90% by mol.

[1521] Propylene Copolymer (A7)

[1522] The propylene copolymer (A7) for constituting the nineteenthpropylene polymer composition is identical with the propylene copolymer(A7) for constituting the thirteenth propylene polymer composition.

[1523] Propylene Polymer (A6)

[1524] The propylene polymer (A6) for constituting the nineteenthpropylene polymer composition is identical with the propylene polymer(A6) for constituting the sixth propylene polymer composition.

[1525] Olefin Elastomer (D)

[1526] The olefin elastomer (D) for constituting the nineteenthpropylene polymer composition is identical with the olefin elastomer (D)for constituting the seventh propylene polymer composition.

[1527] The olefin elastomer (D) can be used in combination of two ormore kinds.

[1528] Olefin Polymer (E)

[1529] The olefin polymer (E) for constituting the nineteenth propylenepolymer composition is identical with the olefin polymer (E) forconstituting the eighth propylene polymer composition.

[1530] The olefin polymer (E) can be used in combination of two or morekinds.

[1531] Propylene Polymer Composition

[1532] The nineteenth propylene polymer composition contains, as itsessential components, the propylene copolymer (A7), the propylenepolymer (A6) which is different from the propylene copolymer (A7), theolefin elastomer (D) and the olefin polymer (E). This compositioncontains the propylene copolymer (A7) in an amount of 5 to 95% byweight, the propylene polymer (A6) in an amount of not more than 95% byweight, the olefin elastomer (D) in an amount of not more than 95% byweight and the olefin polymer (E) in an amount of not more than 95% byweight.

[1533] In the nineteenth propylene polymer composition, it is desiredthat the propylene copolymer (A7) is contained in an amount of 5 to 95%by weight, preferably 30 to 85% by weight, more preferably 30 to 50% byweight; the propylene polymer (A6) is contained in an amount of 2 to 92%by weight, preferably 5 to 60% by weight, more preferably 30 to 50% byweight; the olefin elastomer (D) is contained in an amount of 2 to 92%by weight, preferably 5 to 60% by weight, more preferably 10 to 30% byweight; and the olefin polymer (E) is contained in an amount of 1 to 91%by weight, preferably 5 to 60% by weight, more preferably 10 to 30% byweight.

[1534] In the nineteenth propylene polymer composition, when theintrinsic viscosity ([η]_(A7)) of the propylene copolymer (A7) and theintrinsic viscosity ([η]_(A6)) of the propylene polymer (A6) has arelation of [η]_(A7)≧[η]_(A6), it is desired that [η]_(A7) in the rangeof 1 to 10 dl/g, preferably 2 to 5 dl/g; [η]_(A6) is in the range of 0.2to 1.5 dl/g, preferably 0.3 to 1.0 dl/g; and ([η]_(A7)/[η]_(A6)) is inthe range of 3 to 30, preferably 4 to 20.

[1535] When the intrinsic viscosity ([η]_(A7)) of the propylenecopolymer (A7) and the intrinsic viscosity ([η]_(A6)) of the propylenepolymer (A6) has a relation of [η]_(A7)<[η]_(A6), it is desired that[η]_(A7) is in the range of 0.2 to 1.5 dl/g, preferably 0.3 to 1.0 dl/g;[η]_(A6) is in the range of 1 to 10 dl/g, preferably 2 to 5 dl/g; and([η]_(A6)/[η]_(A7)) is in the range of 3 to 30, preferably 4 to 20.

[1536] The nineteenth propylene polymer composition is desired to haveMFR, as measured at 230° C. under a load of 2.16 kg, of 0.01 to 1,000g/10 min, preferably 0.5 to 200 g/10 min. In this composition, Mw/Mn ofall the propylene components for constituting the composition isdesirably in the range of 4 to 15.

[1537] The density of the nineteenth propylene polymer composition isdesired to be in the range of 0.87 to 0.92 g/cm³, preferably 0.88 to0.92 g/cm³.

[1538] The flexural modulus (FM) thereof is desired to be in the rangeof 2,000 to 20,000 kg/cm², preferably 4,000 to 15,000 kg/cm².

[1539] The Izod impact strength (IZ) thereof at 23° C. is desired to bein the range of 10 to 60 kg·cm/cm, preferably 20 to 60 kg·cm/cm.

[1540] The tensile elongation at break (EL) thereof is desired to be inthe range of 200 to 2,000%, preferably 200 to 1,000%.

[1541] The heat distortion temperature (HDT) thereof is desired to benot lower than 80° C., preferably in the range of 90 to 140° C.

[1542] The nineteenth propylene polymer composition may contain, ifnecessary, additives which may be added to the first propylene polymercomposition, with the proviso that the object of the invention is notmarred.

[1543] The nineteenth propylene polymer composition can be prepared byknown processes. For example, the composition can be prepared inaccordance with the processes (1) to (5) described for the firstpropylene polymer composition, using the propylene copolymer (A7), thepropylene polymer (A6), the olefin elastomer (D) and the olefin polymer(E).

[1544] Such propylene polymer composition is excellent in not only heatresistance, rigidity and tensile elongation at break but alsomoldability and impact resistance.

[1545] The nineteenth propylene polymer composition can be favorablyused for various structural materials such as those of automobiles andelectrical appliances, daily necessaries, various films and sheets.

Effect of the Invention

[1546] The propylene polymer compositions of the invention are excellentin heat resistance, rigidity and tensile elongation at break.

EXAMPLE

[1547] The present invention is described in more detail with referenceto the following examples, but it should be construed that the inventionis in no way limited to those examples.

[1548] In the present invention, physical properties were measured bythe following methods.

[1549] Intrinsic Viscosity [η]

[1550] The intrinsic viscosity [η]was measured in decalin at 135° C.

[1551] Melt Flow Rate (MFR)

[1552] The melt flow rate (MFR) was measured in accordance with ASTMD1238 under the following conditions.

[1553] Conditions: 230° C., 2.16 kg

[1554] Flexural Modulus (FM)

[1555] The flexural modulus (FM) was measured in accordance with ASTMD790 under the following conditions.

[1556] Size of specimen:

[1557] 12.7 (width)×6.4 (thickness)×127 (length)

[1558] Span: 100 mm

[1559] Flexure rate: 2 mm/min

[1560] Izod Impact Strength (IZ)

[1561] The Izod impact strength (IZ) was measured in accordance withASTM D256 under the following conditions.

[1562] Temperature: 23° C., −30° C.

[1563] Size of specimen:

[1564] 12.7 (width)×6.4 (thickness)×64 (length)

[1565] The specimen was mechanically notched.

[1566] Tensile Elongation at Break (EL)

[1567] The tensile elongation at break (EL) was measured in accordancewith ASTM D638 under the following conditions.

[1568] Temperature: 23° C.

[1569] Heat Distortion Temperature (HDT)

[1570] The heat distortion temperature was measured in accordance withASTM D648 under the following conditions.

[1571] Size of specimen:

[1572] 12.7 (width)×6.4 (thickness)×127 (length)

Preparation Example Preparation of a Propylene Polymer (1)

[1573] A catalyst component was prepared by mixing 0.0030 mmol (in termsof Zr atom) of rac-dimethylsilylbis(2-methylindenyl)zirconium dichlorideand 1.50 mmol of methylaluminoxane.

[1574] Into a 4-liter stainless steel autoclave thoroughly purged withnitrogen was introduced 1 liter of purified toluene, followed bystirring for 20 minutes in a propylene atmosphere. Then, the temperatureof the reaction system was raised. When the temperature became 30° C.,1.5 mmol of methylaluminoxane and the catalyst component prepared abovewere added to the system, thereby to perform polymerization for 1 hourat 40° C. under a propylene pressure of 3 kg/cm²-G. After thepolymerization, the solvent was removed by filtration, and the resultingproduct was washed with methanol and dried in vacuo at 80° C. for 10hours.

[1575] Thus, a polymer [propylene polymer (1)] was obtained in an amountof 146 g, and the polymerization activity was 48,700 g-PP/mmol-Zr. Thispolymer had [η] of 2.58 dl/g, MFR of 1.9 g/10 min, Mw of 339,000 andMw/Mn of 2.03.

Preparation of a Propylene Polymer (2)

[1576] Preparation of a Solid Catalyst Component

[1577] A 500-ml reactor thoroughly purged with nitrogen was charged with25 g of silica (i.e., F-948 of Fuji Davison Co. having been dried at200° C. for 6 hours in a stream of nitrogen) and 310 ml of toluene, andthe temperature of the system was made 0° C. with stirring. To thesystem was dropwise added 90 ml of an organoaluminum oxy-compound (i.e.,methylaluminoxane of Schering Co. having been diluted with toluene, 2.1mol/l) over a period of 60 minutes in a nitrogen atmosphere. Then, thereaction was carried out at the same temperature for 30 minutes,successively at 90° C. for 4 hours. Thereafter, the reaction system wascooled by allowing it to stand. When the temperature became 60° C., thesupernatant liquid was removed by decantation, and the resultingreaction liquid was washed three times with 150 ml of toluene.

[1578] Thus, a solid catalyst component (C-1) containing 6.8 mmol of Albased on 1 g of silica was obtained.

[1579] Preparation of a Prepolymerized Catalyst Component (C-2)

[1580] A 500-ml reactor thoroughly purged with nitrogen was charged with320 ml of n-hexane. Then, to the reactor were added 40 mmol (in terms ofAl atom) of the solid catalyst component (C-1) obtained above and 0.04mmol (in terms of Zr atom) ofrac-dimethylsilylbis(2-methylindenyl)zirconium dichloride, and thecontents in the reactor were stirred for 10 minutes. Further, 1.2 mmolof triisobutylaluminum was added, followed by stirring for another 10minutes. Then, a propylene gas (13.4 1/hr) was passed through thereactor for 1 hour at 20° C. to perform prepolymerization of propylene.The supernatant liquid was removed by decantation, and the resultingproduct was washed three times with 150 ml of decane.

[1581] Thus, a prepolymerized catalyst component (C-2) in which Zr andAl were supported in amounts of 0.0042 mmol and 4.35 mmol, respectively,based on 1 g of the solid catalyst was obtained.

[1582] Polymerization

[1583] Into a 4-liter stainless steel autoclave thoroughly purged withnitrogen was introduced 1.5 liters of n-hexane, followed by stirring for20 minutes in a propylene atmosphere. Then, the temperature of thereaction system was raised. When the temperature became 50° C., 2.90mmol of triisobutylaluminum, 0.0030 mmol (in terms of Zr atom) of theprepolymerized catalyst component (C-2) prepared above and 150 ml ofhydrogen were added to the system, thereby to perform polymerization for2 hours at 60° C. under a propylene pressure of 7 kg/cm²-G. After thepolymerization, the solvent was removed by filtration, and the resultingproduct was washed with methanol and dried in vacuo at 80° C. for 10hours.

[1584] Thus, a polymer [propylene polymer (2)] was obtained in an amountof 304 g, and the polymerization activity was 101,000 g-PP/mmol-Zr. Thispolymer had [1] of 1.01 dl/g, MFR of 145 g/10 min and Mw/Mn of 3.78.

Preparation of a Propylene Polymer (3)

[1585] Preparation of a Prepolymerized Catalyst Component (C-3)

[1586] A 500-ml reactor thoroughly purged with nitrogen was charged with350 ml of n-hexane. To the reactor were added 16 mmol (in terms of Alatom) of the solid catalyst component (C-1) prepared above and 0.04 mmol(in terms of Zr atom) of rac-dimethylsilylbis(2-methylindenyl)zirconiumdichloride, and the contents in the reactor were stirred for 10 minutes.Further, 1.2 mmol of triisobutylaluminum was added, followed by stirringfor another 10 minutes. Then, a propylene gas (13.4 1/hr) was passedthrough the reactor for 1 hour at 20° C. to perform prepolymerization ofpropylene. The supernatant liquid was removed by decantation, and theresulting product was washed three times with 150 ml of decane.

[1587] Thus, a prepolymerized catalyst component (C-3) in which Zr andAl were supported in amounts of 0.0011 mmol and 4.50 mmol, respectively,based on 1 g of the solid catalyst was obtained.

[1588] Polymerization

[1589] Into a 2-liter stainless steel autoclave thoroughly purged withnitrogen was introduced 750 ml of n-hexane, followed by stirring for 20minutes in a propylene atmosphere. Then, the temperature of the reactionsystem was raised. When the temperature became 50° C., 2.7 mmol oftriisobutylaluminum and 0.045 mmol (in terms of Zr atom) of theprepolymerized catalyst component (C-3) prepared above were added to thesystem, thereby to perform polymerization for 1.5 hours at 60° C. undera propylene pressure of 7 kg/cm²-G. After the polymerization, thesolvent was removed by filtration, and the resulting product was washedwith methanol and dried in vacuo at 80° C. for 10 hours.

[1590] Thus, a polymer [propylene polymer (3)] was obtained in an amountof 403 g, and the polymerization activity was 89,600 g-PP/mmol-Zr. Thispolymer had [α]of 1.33 dl/g, MFR of 34 g/10 min and Mw/Mn of 2.93.

Preparation of a Propylene Polymer (4)

[1591] Preparation of a Solid Titanium Catalyst Component

[1592] 95.2 g of anhydrous magnesium chloride, 442 ml of decane and390.6 g of 2-ethylhexyl alcohol were mixed and then heated at 130° C.for 2 hours to give a homogeneous solution. To the solution was added21.3 g of phthalic anhydride, and they were further stirred at 130° C.for 1 hour to dissolve the phthalic anhydride in the homogeneoussolution. After the resulting solution was cooled to room temperature,75 ml of the solution was dropwise added to 200 ml of titaniumtetrachloride kept at −20° C. over a period of 1 hour. After theaddition was completed, the temperature of the mixed solution was raisedto 110° C. over a period of 4 hours. When the temperature of thesolution reached 110° C., 5.22 g of diisobutyl phthalate (DIBP) wasadded to the solution, followed by stirring at the same temperature for2 hours. After the 2-hour reaction was completed, the solid portion wascollected by hot filtration, and resuspended in 275 ml of titaniumtetrachloride. The resulting suspension was again heated at 110° C. for2 hours to perform reaction.

[1593] After the reaction was completed, the solid portion was collectedagain by hot filtration, and sufficiently washed with decane and hexaneat 110° C. until any titanium compound liberated in the washing liquidwas not detected. Through the above process, the solid titanium catalystcomponent was obtained in the form of a decane slurry, and a part ofthis decane slurry was dried for the purpose of examining the catalystcomposition.

[1594] As a result, the solid titanium catalyst component had acomposition comprising 2.4% by weight of titanium, 60% by weight ofchlorine, 20% by weight of magnesium and 13.0% by weight of DIBP.

[1595] Preparation of a Prepolymerized Catalyst Component (C-4)

[1596] A 400-ml four-necked glass reactor equipped with a stirrer wascharged with 150 ml of purified hexane, 15 mmol of triethylaluminum, 3mmol of dicyclopentyldimethoxysilane (DCPMS) and 1.5 mmol (in terms ofTi atom) of the solid titanium catalyst component prepared above in anitrogen atmosphere. Then, to the reactor was fed propylene at 20° C.for 1 hour at a feed rate of 3.2 1/hr. After feeding of propylene wascompleted, the reactor was purged with nitrogen, and washing operationconsisting of removal of a supernatant liquid and addition of purifiedhexane was carried out twice. Then, the resulting product wasresuspended in purified hexane, and all the resulting suspension wastransferred into a catalyst bottle to obtain a prepolymerized catalystcomponent (C-4).

[1597] Polymerization

[1598] Into a 17-liter autoclave was introduced 4 kg of propylene atroom temperature in a propylene atmosphere. To the autoclave was added11 liters of hydrogen, and the temperature of the reaction system wasraised to 60° C. To system were further added 5 mmol oftriethylaluminum, 5 mmol of DCPMS and 0.05 mmol (in terms of Ti atom) ofthe prepolymerized catalyst component (C-4) prepared above, and thetemperature of the system was further raised to 70° C. to performpolymerization reaction at the same temperature for 40 minutes.Immediately after the reaction was completed, a small amount of ethanolwas added to the system to decompose the catalyst, thereafter theunreacted propylene and hydrogen were purged. Thus, a white powderypolymer was obtained. The white powdery polymer thus obtained was driedin vacuo at 80° C. for 10 hours.

[1599] The amount of the white powdery polymer [propylene polymer (4)]obtained after drying was 1,630 g, and therefore the polymerizationactivity was 32,600 g-PP/mmol-Ti. This polymer had a boiling heptaneextraction residue proportion (I.I.) of 99.1%, [α]of 3.0 dl/g, MFR of1.2 g/10 min and Mw/Mn of 5.1.

Preparation of a Propylene Polymer (5)

[1600] The procedures of the polymerization and the post treatment forpreparing the propylene polymer (4) were repeated except that theaddition amount of hydrogen was varied to 150 liters.

[1601] The amount of the polymer [propylene polymer (5)] thus obtainedwas 2,030 g, and the polymerization activity corresponded to 40,600g-PP/mmol-Ti. This polymer had [α]of 1.10 dl/g, MFR of 155 g/0.10 min,Mw/Mn of 4.9 and a boiling heptane extraction residue proportion (I.I.)of 97.0%.

Preparation of a Propylene Polymer (6)]

[1602] The procedures of the polymerization and the post treatment forpreparing the propylene polymer (4) were repeated except the additionamount of hydrogen was varied to 60 liters.

[1603] The amount of the polymer [propylene polymer (6)] thus obtainedwas 1,905 g, and the polymerization activity corresponded to 38,100g-PP/mmol-Ti. This polymer had [α]of 1.55 dl/g, MFR of 25 g/10 min,Mw/Mn of 5.0 and a boiling heptane extraction residue proportion (I.I.)of 98.8%.

Preparation of a Propylene Polymer (7))

[1604] Synthesis of 3— (2-biphenylyl)-2-ethylpropionic acid

[1605] To a 2-liter four-necked round flask (equipped with a stirrer, aZimroth condenser, a dropping funnel and a thermometer) were fed 40.4 g(360 mmol) of potassium t-butoxide, 300 ml of toluene and 60 ml ofN-methylpyrrolidone. Then, a solution obtained by dissolving 62.1 g (330mmol) of diethyl ethylmalonate in 150 ml of toluene was dropwise addedto the system while heating at 60° C. in a nitrogen atmosphere. Afterthe addition was completed, the resulting mixture was reacted for 1 hourat the same temperature. Then, to the mixture was dropwise added at thesame temperature a solution obtained by dissolving 60.8 g (300 mmol) of2-phenylbenzyl bromide in 90 ml of toluene. After the addition wascompleted, the temperature of the system was elevated, and the reactionmixture was refluxed for 2 hours. The reaction mixture was poured in 600ml of water, and adjusted to pH 1 by adding 2N—HCl. The organic phasewas separated, and the aqueous phase was extracted three times with 200ml of toluene. The whole organic phase was washed with a saturated saltsolution until the organic phase became neutral, and dried withanhydrous Na₂SO₄. The solvent was concentrated under reduced pressure toobtain 110 g of an yellow-orange concentrated solution.

[1606] To a 2-liter four-necked round flask (equipped with a stirrer, aZimroth condenser, a dropping funnel and a thermometer) were fed 202 g(3.06 mol) of potassium hydroxide and 480 ml of an aqueous solution ofmethanol (methanol/water=4/1 (v/v)). Then, a solution obtained bydissolving the above-obtained concentrate in 150 ml of an aqueoussolution of methanol (methanol/water=4/1 (v/v)) was dropwise added atroom temperature. After the addition, the temperature of the system waselevated, and the resulting mixture was refluxed for 4 hours. Then, themixture was cooled to room temperature, and the precipitated solid wasfiltered. The product obtained by filtration was dissolved in water. Theresulting solution was adjusted to pH 1 (acidic) by adding a sulfuricacid and extracted five times with 200 ml of methylene chloride. Thewhole organic phase was dried with anhydrous Na₂SO₄. The solvent wasconcentrated under reduced pressure to obtain 72.6 g of a white solidproduct.

[1607] To a 1-liter three-necked round flask (equipped with a stirrer, aZimroth condenser and a thermometer) were fed 72.6 g of theabove-obtained white solid, 168 ml of an acetic acid, 111 ml of waterand 39.3 ml of a concentrated sulfuric acid, and the contents in theflask were refluxed for 6 hours in a nitrogen atmosphere. After thereaction was completed, the acetic acid was distilled off under reducedpressure, then to the resulting solution was added 150 ml of water, andthe solution was extracted three times with 150 ml of methylenechloride. The whole organic phase was washed with 150 ml of a saturatedsalt solution, and dried with anhydrous Na₂SO₄. The solvent wasdistilled off under reduced pressure, and the residue was separated andpurified by silica gel chromatography (developed with hexane/ethylacetate (2/1→1/1, by parts by volume)), to obtain 41.1 g of a whitesolid (yield: 54%).

[1608] The physical properties of the product obtained are as follows.

[1609] FD-MS: 254 (M⁺)

[1610] m.p.: 91.2-94.0° C.

[1611] NMR (CDCl₃, 90 MHz) δ=0.71 (t, J 7.2 Hz, 3H, CH₃); 1.16-1.58 (m,2H); 2.32 (bquin, J=7.0 Hz, 1H,

[1612] 2.61-2.99 (m, 2H); 6.89-7.47 (m, 9H)

[1613] IR (KBr disk): 1,696 cm⁻¹ (vc_(c=0))

[1614] Synthesis of 3-(2-biphenylyl)-2-ethylpropionyl chloride

[1615] To a 300-ml three-necked round flask (equipped with a stirrertip, a Zimroth condenser, a thermometer and a NaOH trap) were fed 39.9 g(157.2 mmol) of 3-(2-biphenylyl)-2-ethylpropionic acid and 77.7 ml(1,065 mmol) of thionyl chloride, and the contents in the flask wererefluxed for 2.5 hours in a nitrogen atmosphere. After the reaction wascompleted, the unreacted thionyl chloride was distilled off underreduced pressure to obtain 45.6 g of a coarse product of anyellow-orange liquid. This acid chloride was used for the next reactionwithout any further purification.

[1616] The physical properties of the product obtained are as follows.

[1617] IR (Neat): 1,786 cm⁻¹ (vc_(c=0))

[1618] Synthesis of 4-ethyl-2-phenyl-1-indanone

[1619] To a 500-ml three-necked round flask (equipped with a stirrer, aZimroth condenser, a dropping funnel, a thermometer and a NaOH trap)were fed 24.1 g (181 mmol) of anhydrous aluminum chloride and 150 ml ofcarbon disulfide. Then, a solution obtained by dissolving 45.6 g (52.4mmol) of 3-(2-biphenylyl)-2-ethylpropionyl chloride in 63 ml of carbondisulfide was dropwise added to the system while cooling with ice in anitrogen atmosphere. After the addition was completed, the temperaturein the flask was raised to room temperature to perform reaction for. 1hour. The reaction solution was poured in 600 ml of ice water todecompose the solution, and extracted twice with 300 ml of ether. Thewhole organic phase was successively washed with 300 ml of a saturatedNaHCO₃ solution and 300 ml-of a saturated salt solution, and dried withanhydrous Na₂SO₄. The solvent was distilled off under reduced pressure,and the residue was separated and purified by silica gel chromatography(developed with hexane/ethyl acetate (10/1, by parts by volume)), toobtain 32.4 g of the aimed product as an yellow solid (yield: 88%) Thephysical properties of the product obtained are as follows.

[1620] NMR (CDCl₃, 90 MHz): δ=0.98 (t, J=7.2 Hz, 3H, CH₃); 1.60-2.20 (m,2H); 2.42-2.82 (m, 1H,

[1621] 2.80 (dd, J=3.8 Hz, 16.5 Hz, 1H); 3.36 (dd, J=7.6 Hz, 16.5 Hz,1H); 7.09-7.91 (m, 8H)

[1622] IR (Neat): 1,705 cm⁻¹ (vc_(c=0))

[1623] Synthesis of 2-ethyl-1-hydroxy-2-phenylindane

[1624] To a 500-ml three-necked round flask (equipped with a stirrertip, a Zimroth condenser, a dropping funnel and a thermometer) were fed2.55 g (67.8 mmol) of sodium boron hydride and 84 ml of ethanol. Then, asolution obtained by dissolving 31.8 g (135.3 mmol) of2-ethyl-4-phenyl-1-indanone in 60 ml of ethanol was dropwise added tothe system at room temperature in a nitrogen atmosphere. After theaddition was completed, the temperature of the system was raised to 50°C. to perform reaction for another 3.5 hours. After the reaction, thereaction solution was cooled, and acetone was dropwise added thereto todecompose the unreacted sodium boron hydride. Then, the reaction mixturewas concentrated under reduced pressure, and extracted by the additionof 150 ml of water and 150 ml of ether. After the organic phase wasseparated, the aqueous phase was extracted twice with 100 ml of ether.The whole organic phase was washed with 300 ml of a saturated saltsolution, and dried with anhydrous Na₂SO₄. The solvent was distilled offunder reduced pressure, to obtain 32 g of the aimed product (mixture oftwo kinds of isomers) as a viscous light yellow liquid (yield: 99%).

[1625] The physical properties of the product obtained are as follows.

[1626] NMR (CDCl₃, 90 MHz)=δ=1.02 (t, J=7.1 Hz, 3H, CH₃); 1.31-3.28 (m,5H); 4.86, 5.03 (each d, J=6.4 Hz, 5.1 Hz, respectively, total 1H,

[1627] 7.10-7.66 (m, 8H)

[1628] IR (Neat): 3,340 cm⁻¹ (Vc_(c=0))

[1629] Synthesis of 2-ethyl-4-phenylindene

[1630] To a 1-liter four-necked round flask (equipped with a stirrer, adropping funnel and a thermometer) were fed 29.3 g (123.9 mmol) of2-ethyl-1-hydroxy-4-phenylindane, 51.6 g (371.4 mmol) of triethylamine,0.75 g (6.3 mmol) of 4-dimethylaminopyridine and 294 ml of methylenechloride. Then, a solution obtained by dissolving 19.2 ml (247.5 mmol)of methanesulfonyl chloride in 19.5 ml of methylene chloride wasdropwise added slowly to the system while cooling with ice in a nitrogenatmosphere. After the addition was completed, the resulting mixture wasreacted for another 3.5 hours at the same temperature. The reactionmixture was poured in 500 ml of ice water, then the organic phase wasseparated, and the aqueous phase was further extracted twice with 150 mlof methylene chloride. The whole organic phase was successively washedwith a saturated NaHCO₃ solution and a saturated salt solution, anddried with anhydrous Na₂SO₄. The solvent was distilled off under reducedpressure, and the residue was separated by silica gel chromatography(developed with hexane), to obtain 19.7 g of the aimed product (mixtureof two kinds of isomers) as a light yellow liquid (yield: 73%) Thephysical properties of the product obtained are as follows.

[1631] NMR (CDCl₃, 90 MHz): 6=1.20 (t, J=7.6 Hz, 3H, CH₃); 2.49 (q,J=7.6 Hz, 2H); 3.41 (s, 2H); 6.61, 6.72 (each bs, total 1H); 7.09-8.01(m, 8H)

[1632] Synthesis of dimethylsilyl-bis(2-ethyl-4-phenylindene)

[1633] To a 500-ml three-necked round flask (equipped with a stirrertip, a Zimroth condenser, a dropping funnel and a thermometer) were fed.15 g (68.4 mmol) of 2-ethyl-4-phenylindene, 240 mg (1.89 mmol) of copperthiocyanate and 150 ml of anhydrous ether. Then, 47.1 ml (75.3 mmol) ofa hexane solution of n-butyllithium having a concentration of 1.6 M wasdropwise added slowly to the system while cooling with ice in a nitrogenatmosphere. After the addition was completed, the temperature of thesystem was raised to room temperature to perform reaction for another 1hour. Then, 0.5 to the reaction mixture was dropwise added slowly asolution obtained by 4.56 ml (37.8 mmol) of dimethyldichlorosilane in13.5 ml of anhydrous ether. After the addition was completed, themixture was further reacted for 12 hours at room temperature. Thereaction mixture was filtered with Celite, and the filtrate was pouredin 150 ml of saturated ammonium chloride water. After the organic phasewas separated, the aqueous phase was extracted with 150 ml of ether. Thewhole organic phase was washed with a saturated salt solution, and driedwith anhydrous Na₂SO₄. The solvent was distilled off under reducedpressure, and the residue was separated by silica gel chromatography(developed with hexane→hexane/methylene chloride (20/1, by parts byvolume)), to obtain 13.5 g of the aimed product (mixture of two kinds ofisomers) as a light yellow solid (yield: 80%)

[1634] The physical properties of the product obtained are as follows.

[1635] NMR (CDCl₃, 90 MHz): δ=−0.23, −0.17 (each s, total 6H, S₁—CH₃);1.12, 1.19 (each t, each J=7.4 Hz, total 6H, CH₃); 2.44 (bq, J=7.4 Hz,4H); 3.81 (s, 2H,

[1636] 6.75 (bs, 2H, 0.3-H-Ind); 6.88-7.74 (m, 16H)

[1637] Synthesis ofrac-dimethylsilyl-bis(2-ethyl-4-phenylindenyl)zirconium dichloride

[1638] To a 200-ml three-necked round flask (equipped with a stirrertip, a ball condenser, a dropping funnel and a thermometer) were fed2.52 g (5.07 mmol) of dimethylsilyl-bis(2-ethyl-4-phenylindene) and 51ml of anhydrous ether in an argon atmosphere. Then, 6.75 ml (10.68 mmol)of a hexane solution of n-butyllithium having a concentration of 1.58 Mwas dropwise added slowly to the system at room temperature. After theaddition, the resulting mixture was further reacted for 13.5 hours. Thereaction solution was cooled in a dry ice-acetone bath to −70° C., andthereto was slowly added 1.185 g (5.07 mmol) of a ZrCl₄ powder. Afterthe addition was completed, the mixture was left overnight withstirring. Then, the solvent was distilled off at room temperature underreduced pressure. After addition of 90 ml of methylene chloride, theinsolubles were filtered and the filtrate was concentrated at roomtemperature to give a solid. The solid was filtered, then washed twicewith 5 ml of anhydrous ether, and dried under reduced pressure to obtain0.68 g of the aimed product as an orange-yellow solid (yield: 20%)

[1639] The physical properties of the product obtained are as follows.

[1640] NMR (CDCl₃, 90 MHz) δ=1.09 (t, J=7.3 Hz, 6H, CH₃) 1.34 (s, 6H,S₁—CH₃); 2.46 (quin, J=7.3 Hz, 2H); 2.73 (quin, J=7.3 Hz, 2H); 6.96 (s,2H, 3-H-Ind); 6.99-7.88 (m, 16H)

[1641] Polymerization

[1642] To a 100-liter stainless steel polymerizer was fed 50 liters oftoluene in a nitrogen atmosphere, and the system was cooled to 0° C.Then, propylene and hydrogen were fed to the system for 2 hours at feedrates of 4 Nm³/hr and 400 Nl/hr, respectively, to saturate the systemsufficiently. After the feed rate of propylene was reduced to 2 Nm³/hr,to the system were added 15.0 mmol of triisobutylaluminum, 30.0 mmol (interms of Al atom) of methylaluminoxane and 0.10 mmol (in terms of Zratom) of rac-dimethylsilyl-bis(2-ethyl-4-phenylindenyl)zirconiumdichloride to-perform polymerization for 1 hour while keeping the systemat 0° C. The polymerization was terminated by adding 0.5 liter ofmethanol to the system. The resulting polymer suspension was allowed tostand for 6 hours while purging the system with nitrogen. Then, about ahalf amount of toluene was taken out by decantation, and the remainingpolymer suspension was transferred into a 200-liter reactor containingtherein 0.1 liter of a hydrochloric acid and 60 liters of methanol,followed by stirring for 30 minutes.

[1643] After the polymer suspension was allowed to stand and subjectedto decantation, the suspension was again subjected to washing with 50liters of methanol and decantation. Then, the polymer suspension wastaken out from the bottom of the reactor, and the solvent was separatedby filtration. The resulting polymer was dried at 100° C. under highvacuum for one day.

[1644] The amount of the propylene homopolymer [propylene polymer (7)]obtained was 1,950 g, and the polymerization activity corresponded to19,500 g-PP/mmol-Zr. This polymer had [η] of 0.68 dl/g, MFR of 900 g/10min and Mw/Mn of 2.02. In this polymer, the triad tacticity was 99.5%,the proportion of the irregularly positioned units based on the2,1-insertion of the propylene monomer was 0.11%, and the proportion ofthe irregularly positioned units based on the 1,3-insertion of thepropylene monomer was below the detected lower limit (less than 0.03%)

(Preparation of a Propylene Polymer (8)

[1645] The procedures of the polymerization and the post treatment forpreparing the propylene polymer (7) described above were repeated exceptthat the feed rate of hydrogen was varied to 90 Nl/hr.

[1646] The amount of the propylene homopolymer (propylene polymer (8))thus obtained corresponded to 2,720 g, and the polymerization activitycorresponded to 27,200 g-PP/mmol-Zr. This polymer had [η] of 3.25 dl/g,MFR of 0.75 g/10 min and Mw/Mn of 2.20. In this polymer, the triadtacticity was 99.6%, the proportion of the irregularly positioned unitsbased on the 2,1-insertion of the propylene monomer was 0.16%, and theproportion of the irregularly positioned units based on the1,3-insertion of the propylene monomer was below the detected lowerlimit (less than 0.03%)

[1647] Preparation of a Propylene Polymer (9)

[1648] The procedures of the polymerization and the post treatment forpreparing the propylene polymer (7) described above were repeated exceptthat the feed rate of hydrogen was varied to 120 Ni/hr.

[1649] The amount of the propylene homopolymer [propylene polymer (9)]thus obtained was 3,350 g, and the polymerization activity correspondedto 33,500 g-PP/mmol-Zr. This polymer had [η]of 1.64 dl/g, MFR of 13.5g/10 min and Mw/Mn of 2.03. In this polymer, the triad tacticity was99.5%, the proportion of the irregularly positioned units based on the2,1-insertion of the propylene monomer was 0.13%, and the proportion ofthe irregularly positioned units based on the 1,3-insertion of thepropylene monomer was below the detected lower limit (less than 0.03%)

Preparation of a Propylene Polymer (10)

[1650] The procedures of the polymerization and the post treatment forpreparing the propylene polymer (4) described above were repeated exceptthat the addition amount of hydrogen was varied to 45 liters.

[1651] The amount of the propylene homopolymer [propylene polymer (10)]thus obtained was 1,930 g, and the polymerization activity correspondedto 38,600 g-PP/mmol-Ti. This polymer had [η] of 1.75 dl/g, MFR of 15g/10 min, Mw/Mn of 5.0 and a boiling heptane extraction residueproportion (I.I.) of 98.8%.

Preparation of a Propylene Polymer (11)

[1652] The procedures of the polymerization and the post treatment forpreparing the propylene polymer (7) described above were repeated exceptthat the feed rate of hydrogen was varied to 350 Nl/hr.

[1653] The amount of the propylene homopolymer [propylene polymer (11)]thus obtained was 2,060 g, and the polymerization activity correspondedto 20,600 g-PP/mmol-Zr. This polymer had [η] of 0.72 dl/g, MFR of 670g/10 min and Mw/Mn of 1.95. In this polymer, the triad tacticity was99.5%, the proportion of the irregularly positioned units based on the2,1-insertion of the propylene monomer was 0.14%, and the proportion ofthe irregularly positioned units based on the 1,3-insertion of thepropylene monomer was below the detected lower limit (less than 0.03%)

Preparation of a Propylene Polymer (12)

[1654] To a 100-liter stainless steel polymerizer was fed 50 liters oftoluene, and the system was cooled to 0° C. Then, propylene, ethyleneand hydrogen were fed to the system for 2 hours at feed rates of 4Nm³/hr, 2 Nm³/hr and 10 Nl/hr, respectively, to saturate the systemsufficiently. The feed rates of propylene and ethylene were reduced to 1Nm³/hr and 300 Nl/hr, respectively, and the system was allowed to standfor 1 hour. Then, to the system were added 8.0 mmol oftriisobutylaluminum, 12.0 mmol (in terms of Al atom) ofmethylaluminoxane and 0.040 mmol (in terms of Zr atom) ofrac-dimethylsilyl-bis(2-ethyl-4-phenylindenyl)zirconium dichloride, toperform polymerization for 1 hour while keeping the system at 0° C. Thetermination of the polymerization and the post treatment were carriedout in the same manner as described for the propylene polymer (7).

[1655] The amount of the propylene copolymer [propylene polymer (12)]thus obtained was 1,550 g, and the polymerization activity correspondedto 38,700 g-polymer/mmol-Zr. This polymer had [η] of 0.68 dl/g, MFR of950 g/10 min and Mw/Mn of 2.33, and contained constituent units derivedfrom ethylene in an amount of 5.1% by mol. In this polymer, the triadtacticity was-99.2%, the proportion of the irregularly positioned unitsbased on the 2,1-insertion of the propylene monomer was 0.08%, and theproportion of the irregularly positioned units based on the1,3-insertion of the propylene monomer was below the detected lowerlimit (less than 0.03%)

Preparation of a Propylene Polymer (13)

[1656] To a 100-liter stainless steel polymerizer was fed 35 liters oftoluene, and the system was cooled to 0° C.

[1657] Then, propylene and ethylene were fed to the system for 2 hoursat feed rates of 4 Nm³/hr and 2 Nm³/hr, respectively, while adjustingthe pressure in the system at 2.5 kg/cm²-G, so as to saturate the systemsufficiently. The feed rates of propylene and ethylene were reduced to 1Nm³/hr and 300 Nl/hr respectively, and the system was allowed to standfor 1 hour. Then, to the system were added 5.0 mmol oftriisobutylaluminum, 10.0 mmol (in terms of Al atom) ofmethylaluminoxane and 0.010 mmol (in terms of Zr atom) ofrac-dimethylsilyl-bis(2-ethyl-4-phenylindenyl)zirconium dichloride, toperform polymerization for 1 hour at 0° C. while adjusting the pressurein the polymerizer at 2.5 kg/cm²-G. After the polymerization wasterminated by methanol, the pressure in the system was released, and thesystem was purged with nitrogen. The post treatment was carried out inthe same manner as described for the propylene polymer (7).

[1658] The amount of the propylene copolymer [propylene polymer (13)]thus obtained was 1,310 g, and the polymerization activity correspondedto 13,100 g-polymer/mmol-Zr. This polymer had [η]of 3.10 dl/g, MFR of0.72 g/10 min and Mw/Mn of 2.3, and contained constituent units derivedfrom ethylene in an amount of 5.6% by mol. In this polymer, the triadtacticity was 99.3%, the proportion of the irregularly positioned unitsbased on the 2,1-insertion of the propylene monomer was 0.13%, and theproportion of the irregularly positioned units based on the1,3-insertion of the propylene monomer was below the detected lowerlimit (less than 0.03%)

Preparation of a Propylene Polymer (14)

[1659] The procedures of the polymerization and the post treatment forpreparing the propylene polymer (12) described above were repeatedexcept that hydrogen was not used.

[1660] The amount of the propylene copolymer (propylene polymer (14)]thus obtained was 1,750 g, and the polymerization activity correspondedto 17,500 g-polymer/mmol-Zr. This polymer had [ ]) of 1.67 dl/g, MFR of9.5 g/10 min and Mw/Mn of 2.10, and contained constituent units derivedfrom ethylene in an amount of 5.6% by mol. In this polymer, the triadtacticity was 99.2%, the proportion of the irregularly positioned unitsbased on the 2,1-insertion of the propylene monomer was 0.11%, and theproportion of the irregularly positioned units based on the1,3-insertion of the propylene monomer was below the detected lowerlimit (less than 0.03%)

Preparation of a Soft Polymer (Ethylene/Propylene Random Copolymer)

[1661] Preparation of a Solid Titanium Catalyst Component

[1662] 23.8 g of anhydrous magnesium chloride, 122 ml of decane and116.1 g of 2-ethylhexyl alcohol were together heated at 130° C. for 2hours to give a homogeneous solution. To the solution was added 5.72 mlof ethyl benzoate. The resulting homogeneous solution was dropwise addedto 1 liter of titanium tetrachloride kept at −20° C. over a period of 20minutes with stirring, and the resulting solution was further stirredfor 1 hour at −20° C. Then, the temperature of the solution was slowlyraised. When the temperature of the solution reached 80° C., 12.2 ml ofethyl benzoate was further added to the solution, and the mixture wasstirred for 2 hours at 80° C.

[1663] After the reaction was completed, the solid material wascollected by filtration. The solid material was resuspended in 1 literof titanium tetrachloride, and the suspension was stirred for 2 hours at90° C. The solid material was again collected by filtration and washedsufficiently with purified hexane until any titanium compound liberatedin the washing liquid was not detected.

[1664] The solid titanium catalyst component thus obtained containedtitanium, chlorine, magnesium and ethyl benzoate in amounts of 3.7% byweight, 59% by weight, 17% by weight and 15% by weight, respectively.

[1665] Polymerization

[1666] In a 15-liter stainless steel polymerizer equipped with astirrer, copolymerization of ethylene and propylene was carried out.

[1667] To the polymerizer were continuously fed, through the topthereof, hexane as a polymerization solvent at a feed rate of 3 1/hr, ahexane slurry of the solid titanium catalyst component obtained above(0.15 mmol/l in terms of titanium atom) at a feed rate of 1 1/hr, ahexane solution of triethylaluminum (15 mmol/l) at a feed rate of 0.51/hr and a hexane solution of ethyl benzoate (5 mmol/l) at a feed rateof 0.5 1/hr. Further, to the polymerizer were continuously fed, throughthe top thereof, ethylene at a feed rate of 90 1/hr and propylene at afeed rate of 270 1/hr, and was also continuously fed hydrogen so thatthe hydrogen concentration in the gas phase of the polymerizer was 2.3%.

[1668] On the other hand, the polymer solution was continuously drawnout from the bottom of the polymerizer so that the amount of the polymersolution in the polymerizer was 5 liters.

[1669] The copolymerization was carried out at 80° C. by circulatingwarm water within a jacket equipped on the outside of the polymerizer.The pressure in the polymerizer was 6.5 kg/cm²-G.

[1670] To the polymer solution drawn out from the polymerizer was addeda small amount of methanol to terminate the polymerization reaction. Thepolymer solution was subjected to steam stripping to separate thepolymer from the solvent, and the polymer was dried at 80° C. underreduced pressure for one day.

[1671] Through the above operation, an ethylene/propylene randomcopolymer (EPR-1) was obtained in an amount of 235 g/hr.

[1672] The ethylene/propylene random copolymer (EPR-1) containedconstituent units derived from ethylene in an amount of 42% by mol, andhad [α]of 2.7 dl/g.

Preparation of an Ethylene/Propylene Random Copolymer (EPR-2)

[1673] In a 15-liter autoclave equipped with a stirrer, copolymerizationof ethylene and propylene was carried out.

[1674] To the polymerizer were fed, through the top thereof, 2.4 litersof dehydrated and purified hexane, 3.3 kg of propylene, 0.72 ml of atoluene solution of methylaluminoxane (1.3 mg-atom/ml in terms ofaluminum atom) and 7.7 ml of a hexane solution of triisobutylaluminum (1mmol/ml).

[1675] After the temperature of the system was raised to 37° C.,ethylene was fed to the system so that the total pressure was 14 kg/cm²,and 2.4 ml of a toluene solution ofbis(1,3-dimethylcyclopentadienyl)zirconium dichloride (0.004 mmol/ml)was fed to the system using a pressure equalizing tube. Thepolymerization was performed for 1 hour with keeping the temperature at37° C. and the total pressure at 14 kg/cm². After release of pressure,the polymer solution was taken out and dried. An yield of the resultingpolymer was 320 g.

[1676] The ethylene/propylene random copolymer (EPR-2) thus obtainedcontained constituent units derived from ethylene in an amount of 43% bymol, and had [η] of 2.8 dl/g.

Synthesis of an Ethylene/Propylene Random Copolymer (EPR-3)

[1677] In a 2-liter autoclave equipped with a stirrer, copolymerizationof ethylene and propylene was carried out.

[1678] In detail, to the autoclave were fed, through the top thereof,0.9 liter of dehydrated and purified hexane, 1 ml of a hexane solutionof triisobutylaluminum (1 mmol/ml) and 0.27 ml of a toluene solution ofmethylaluminoxane. (0.9 mmol/ml in terms of Al atom). After thetemperature of the system was raised to 50° C., propylene was fed to thesystem so that the total pressure was 3.8 kg/cm²-G, and ethylene wasfurther fed to the system so that the total pressure was 8 kg/cm²-G.Then, to the system was added 0.0008 mmol (in terms of zirconium) ofrac-dimethylsilyl-bis(2-ethyl-4-phenylindenyl)zirconium dichloride toperform polymerization for 30 minutes with keeping the temperature at50° C. and the total pressure at 8 kg/cm². After release of pressure,the polymer solution was added to a large amount of methanol. Theresulting polymer was taken out and dried at 130° C. for 12 hours underreduced pressure.

[1679] An yield of the ethylene/propylene random copolymer (EPR-3) thusobtained was 49.6 g. This copolymer contained constituent units derivedfrom ethylene in an amount of 39% by mol, and had [η] of 3.1 dl/g andMFR of 0.4 g/10 min.

Synthesis of an Ethylene/Propylene Random Copolymer (EPR-4)

[1680] An ethylene/propylene random copolymer (EPR-4) was synthesized bya conventional ethylene/propylene copolymerization process using aVO(OC₂H₅)Cl₂—(C₂H₅)_(1.5)AlCl_(1.5) catalyst.

[1681] The ethylene/propylene random copolymer (EPR-4) thus obtained had[η]of 2.4 dl/g and MFR of 0.6 g/10 min, and contained constituent unitsderived from ethylene in an amount of 81% by mol.

Synthesis of an Ethylene/Propylene Random Copolymer (EPR-5)

[1682] In a 2-liter autoclave equipped with a stirrer, copolymerizationof ethylene and propylene was carried out.

[1683] In detail, to the polymerizer were fed, through the top thereof,1 liter of dehydrated and purified hexane, 11 Nl of propylene in theform of a gas, 0.85 ml of a hexane solution of triisobutylaluminum (1mmol/ml) and 0.13 ml of a toluene solution of methylaluminoxane (1.2mmol/ml in terms of Al atom). After the temperature of the system wasraised to 80° C., ethylene was fed to the system so that the totalpressure was 8 kg/cm²-G. Then, to the system was added 0.0005 mmol (interms of Zr atom) ofrac-dimethylsilyl-bis(2-ethyl-4-phenylindenyl)zirconium dichloride toperform polymerization for 30 minutes with keeping the temperature at80° C. and the total pressure at 8 kg/cm²-G. After release of pressure,the polymer solution was added to a large amount of methanol. Theresulting polymer was taken out and dried at 130° C. for 12 hours underreduced pressure.

[1684] An yield of the ethylene/propylene random copolymer (EPR-5) thusobtained was 58.4 g. This copolymer contained constituent units derivedfrom ethylene in an amount of 79% by mol, and had [η] of 2.2 dl/g andMFR of 0.7 g/10 min.

Synthesis of an Ethylene/1-Butene Random Copolymer (EBR-1)

[1685] In a 2-liter autoclave equipped with a stirrer, copolymerizationof ethylene and 1-butene was carried out.

[1686] In detail, to the polymerizer were fed, through the top thereof,1 liter of dehydrated and purified hexane, 55 ml of 1-butene, 0.85 ml ofa hexane solution of triisobutylaluminum (1 mmol/ml) and 0.13 ml of atoluene solution of methylaluminoxane (1.2 mmol/ml in terms of Al atom).After the temperature of the system was raised to 90° C., ethylene wasfed to the system so that the total pressure was 8 kg/cm²-G. Then, tothe system was added 0.0005 mmol (in terms of Zr atom) ofrac-dimethylsilyl-bis(2-ethyl-4-phenylindenyl)zirconium dichloride toperform polymerization for 20 minutes with keeping the temperature at90° C. and the total pressure at 8 kg/cm²-G. After release of pressure,the polymer solution was added to a large amount of methanol. Theresulting polymer was taken out and dried at 130° C. for 12 hours underreduced pressure.

[1687] An yield of the ethylene/1-butene random copolymer (EBR-5) thusobtained was 52.8 g. This copolymer contained constituent units derivedfrom ethylene in an amount of 82% by mol, and had [η] of 2.3 dl/g andMFR of 0.6 g/10 min.

Synthesis of Ethylene Polymers (PE-1) and (PE-2)

[1688] Ethylene polymers (PE-1) and (PE-2) were synthesized by aconventional ethylene copolymerization process using a combined catalystof MgCl₂-supported Ti catalyst-triethylaluminum.

[1689] The ethylene polymer (PE-1) had [η] of 1.20 dl/g, MFR of 29 g/10min and Mw/Mn of 4.1.

[1690] The ethylene polymer (PE-2) had [η] of 2.11 dl/g, MFR of 1.3 g/10min and Mw/Mn of 4.8.

Example 1

[1691] A propylene polymer composition consisting of 40% by weight ofthe propylene polymer (1) and 60% by weight of the propylene polymer (2)prepared by the above polymerization was molded into ASTM specimens bymeans of an injection molding machine under the conditions of a resintemperature of 200° C. and a mold temperature of 40° C., to measure thephysical properties.

[1692] The results are set forth in Table 1.

[1693] Comparative Example 1

[1694] The propylene polymer (3) prepared by the above polymerizationwas molded into ASTM specimens in the same manner as described inExample 1, to measure the physical properties.

[1695] The results are set forth in Table 1.

Comparative Example 2

[1696] A propylene polymer composition consisting of 40% by weight ofthe propylene polymer (4) and 60% by weight of the propylene polymer (5)prepared by the above polymerization was molded into ASTM specimens inthe same manner as described in Example 1, to measure the physicalproperties.

[1697] The results are set forth in Table 1. TABLE 1 Ex. 1 Comp. Ex. 1Comp. Ex. 2 Propylene polymer (1) 40 — — Propylene polymer (2) 60 — —Propylene polymer (3) — 100 — Propylene polymer (4) — — 40 Propylenepolymer (5) — — 60 MFR (g/10 min) 20 31 18 FM (kg/cm²) 15,000 11,10019,500 IZ (23° C.) (kg · cm/cm) 2 2 2 EL (%) 420 340 30 HDT (load: 4.6kg) (° C.) 110 94 117

Example 2

[1698] A propylene polymer composition consisting of 40 parts by weightof the propylene polymer (1), 60 parts by weight of the propylenepolymer (2) and 20 parts by weight of the soft polymer (EPR-1) preparedby the above polymerization was molded into ASTM specimens in the samemanner as described in Example 1, to measure the physical properties.

[1699] The results are set forth in Table 2.

Comparative Example 3

[1700] A propylene polymer composition consisting of 100 parts by weightof the propylene polymer (3) and 20 parts by weight of the soft polymer(EPR-1) prepared by the above polymerization was molded into ASTMspecimens in the same manner as described in Example 1, to measure thephysical properties.

[1701] The results are set forth in Table 2.

Comparative Example 4

[1702] A propylene polymer composition consisting of 40 parts by weightof the propylene polymer (4), 60 parts by weight of thepropylene-polymer (5) and 20 parts by weight of the soft polymer (EPR-1)prepared by the above polymerization was molded into ASTM specimens inthe same manner as described in Example 1, to measure the physicalproperties.

[1703] The results are set forth in Table 2. TABLE 2 Ex. 2 Comp. Ex. 3Comp. Ex. 4 Propylene polymer (1) 40 — — Propylene polymer (2) 60 — —Propylene polymer (3) — 100 — Propylene polymer (4) — — 40 Propylenepolymer (5) — — 60 Soft polymer 20 20 20 MFR (g/10 min) 15 25 12 FM(kg/cm²) 11,000 9,100 13,000 IZ (23° C.) (kg · cm/cm) 35 37 12 EL (%)720 740 180 HDT (load: 4.6 kg) (° C.) 95 88 110

Example 3

[1704] A propylene polymer composition consisting of 50% by weight ofthe propylene polymer (4) and 50% by weight of the propylene polymer (5)prepared by the above polymerization was molded into ASTM specimens inthe same manner as described in Example 1, to measure the physicalproperties.

[1705] The results are set forth in Table 3.

Comparative Example 5

[1706] A propylene polymer composition consisting of 50% by weight ofthe propylene polymer (4) and 50% by weight of the propylene polymer (5)prepared by the above polymerization was molded into ASTM specimens inthe same manner as described in Example 1, to measure the physicalproperties.

[1707] The results are set forth in Table 3. TABLE 3 Ex. 3 Comp. Ex. 5Propylene polymer (4) 50 50 Propylene polymer (2) 50 — Propylene polymer(5) — 50 MFR (g/10 min) 15 15 FM (kg/cm²) 18,000 19,000 IZ (23° C.) (kg· cm/cm) 2 2 EL (%) 180 28 HDT (load: 4.6 kg) (° C.) 115 115

Example 4

[1708] A propylene polymer composition consisting of 50 parts by weightof the propylene polymer (4), 50 parts by weight of the propylenepolymer (2) and 20 parts by weight of the soft polymer (EPR-1) preparedby the above polymerization was molded into ASTM specimens in the samemanner as described in Example 1, to measure the physical properties.

[1709] The results are set forth in Table 4.

Comparative Example 6

[1710] A propylene polymer composition consisting of 50 parts by weightof the propylene polymer (4), 50 parts by weight of the propylenepolymer (5) and 20 parts by weight of the soft polymer (EPR-1) preparedby the above polymerization was molded into ASTM specimens in the samemanner as described in Example 1, and to measure the physicalproperties.

[1711] The results are set forth in Table 4. TABLE 4 Ex. 4 Comp. Ex. 6Propylene polymer (4) 50 50 Propylene polymer (2) 50 — Propylene polymer(5) — 50 Soft polymer 20 20 MFR (g/10 min) 12 15 FM (kg/cm²) 12,50013,000 IZ (23° C.) (kg · cm/cm) 30 12 EL (%) 400 180 HDT (load: 4.6 kg)(° C.) 95 105

Example 5

[1712] A propylene polymer composition consisting of 100 parts by weightof the propylene polymer (6) and 20 parts by weight of theethylene/propylene random copolymer (EPR-2) prepared by the abovepolymerization was molded into ASTM specimens in the same manner asdescribed in Example 1, to measure the physical properties.

[1713] The results are set forth in Table 5.

Comparative Example 7

[1714] A propylene polymer composition consisting of 100 parts by weightof the propylene polymer (6) and 20 parts by weight of theethylene/propylene random copolymer (EPR-1) prepared by the abovepolymerization was molded into ASTM specimens in the same manner asdescribed in Example 1, to measure the physical properties.

[1715] The results are set forth in Table 5. TABLE 5 Ex. 5 Comp. Ex. 7Propylene polymer (6) 100 100 EPR-2 20 — EPR-1 — 20 MFR (g/10 min) 17 17FM (kg/cm²) 13,100 13,300 IZ (23° C.) (kg · cm/cm) 18 12 IZ (−30° C.)(kg · cm/cm) 8 3 EL (%) 350 250 HDT (load: 4.6 kg) (° C.) 95 95

Example 6

[1716] A propylene polymer composition consisting of 50 parts by weightof the propylene polymer (7) and 50 parts by weight of the propylenepolymer (8) prepared by the above polymerization was molded into ASTMspecimens in the same manner as described in Example 1, to measure thephysical properties.

[1717] The results are set forth in Table 6.

Comparative Example 8

[1718] The propylene polymer (9) prepared by the above polymerizationwas molded into ASTM specimens in the same manner as described inExample 1, to measure the physical properties.

[1719] The results are set forth in Table 6. TABLE 6 Ex. 6 Comp. Ex. 8Propylene polymer (7) 50 — Propylene polymer (8) 50 — Propylene polymer(9) — 100 MFR (g/10 min) 12.3 13.5 FM (kg/cm²) 18,200 17,000 IZ (23° C.)(kg · cm/cm) 2.1 3.4 EL (%) 380 340 HDT (load: 4.6 kg) (° C.) 128 125

Example 7

[1720] A propylene polymer composition consisting of 50 parts by weightof the propylene polymer (12) and 50 parts by weight of the propylenepolymer (13) prepared by the above polymerization was molded into ASTMspecimens in the same manner as described in Example 1, to measure thephysical properties. Further, a film was produced from the abovecomposition under the following conditions, to measure the haze.

[1721] The film (width: 30 cm, thickness: 50 μm) was produced by meansof a single-screw extruder having a diameter of 30 mm equipped with aT-die under the conditions of a cooling roll temperature of 25° C. and atake-up rate of 3 m/min.

[1722] The results are set forth in Table 7.

Comparative Example 9

[1723] The propylene polymer (14) prepared by the above polymerizationwas molded into ASTM specimens, to measure the physical properties.

[1724] The results are set forth in Table 7. TABLE 7 Ex. 7 Comp. Ex. 9Propylene polymer (12) 50 — Propylene polymer (13) 50 — Propylenepolymer (14) — 100 MFR (g/10 min) 13.0 9.5 FM (kg/cm²) 8,200 7,700 IZ(23° C.) (kg · cm/cm) 4.0 4.6 EL (%) 440 480 Film haze (%) 0.7 2.0

Example 8

[1725] A propylene polymer composition consisting of 50 parts by weightof the propylene polymer (4) and 50 parts by weight of the propylenepolymer (11) prepared by the above polymerization was molded into ASTMspecimens in the same manner as described in Example 1, to measure thephysical 1.0 properties.

[1726] The results are set forth-in Table 8.

Comparative Example 10

[1727] A propylene polymer composition consisting of 50 parts by weightof the propylene polymer (4) and 50 parts by 15 weight of the propylenepolymer (5) prepared by the above polymerization was molded into ASTMspecimens in the same manner as described in Example 1, to measure thephysical properties.

[1728] The results are set forth in Table 8. TABLE 8 Ex. 8 Comp. Ex. 10Propylene polymer (4) 50 50 Propylene polymer (11) 50 — Propylenepolymer (5) — 50 MFR (g/10 min) 16 15 FM (kg/cm²) 19,000 19,000 IZ (23°C.) (kg · cm/cm) 2 2 EL (%) 280 28 HDT (load: 4.6 kg) (° C.) 118 115

Example 9

[1729] A propylene polymer composition consisting of 50 parts by weightof the propylene polymer (7), 50 parts by weight of the propylenepolymer (8) and 20 parts by weight of the ethylene/propylene randomcopolymer (EPR-1) prepared by the above polymerization was molded intoASTM specimens in the same manner as described in Example 1, to measurethe physical properties.

[1730] The results are set forth in Table 9.

Example 10

[1731] A propylene polymer composition consisting of 50 parts by weightof the propylene polymer (7), 50 parts by weight of the propylenepolymer (8), 10 parts by weight of the ethylene/propylene randomcopolymer (EPR-3) and 10 parts by weight of the ethylene/propylenerandom copolymer (EPR-5) prepared by the above polymerization was moldedinto ASTM specimens in the same manner as described in Example 1, tomeasure the physical properties.

[1732] The results are set forth in Table 9. TABLE 9 Ex. 9 Ex. 10Propylene polymer (7) 50 50 Propylene polymer (8) 50 50 EPR-1 20 — EPR-3— 10 EPR-5 — 10 MFR (g/10 min) 9.1 9.1 FM (kg/cm²) 12,800 13,600 IZ (23°C.) (kg · cm/cm) 38 34 EL (%) 720 560 HDT (load: 4.6 kg) (° C.) 98 104

Example 11

[1733] A propylene polymer composition consisting of 50 parts by weightof the propylene polymer (12), 50 parts by weight of the propylenepolymer (13) and 20 parts by weight of the ethylene/propylene randomcopolymer (EPR-1) prepared by the above polymerization was molded intoASTM specimens in the same manner as described in Example 1, to measurethe physical properties. Further, a film was produced from the abovecomposition in the same manner as described in Example 7, to measure thehaze.

[1734] The results are set forth in Table 10.

Comparative Example 11

[1735] A propylene polymer composition consisting of 100 parts by weightof the propylene polymer (14) and 20 parts by weight of theethylene/propylene random copolymer (EPR-1) prepared by the abovepolymerization was molded into ASTM specimens in the same manner asdescribed in Example 1, to measure the physical properties. Further, afilm was produced from the above composition in the same manner asdescribed in Example 7, to measure the haze.

[1736] The results are set forth in Table 10. TABLE 10 Ex. 11 Comp. Ex.11 Propylene polymer (12) 50 — Propylene polymer (13) 50 — Propylenepolymer (14) — 100 EPR-1 20 20 MFR (g/10 min) 13.0 7.2 FM (kg/cm²) 6,2005,600 IZ (23° C.) (kg · cm/cm) 38 46 EL (%) 520 540 Film haze (%) 0.72.0

Example 12

[1737] A propylene polymer composition consisting of 50 parts by weightof the propylene polymer (4), 50 parts by weight of the propylenepolymer (11) and 20 parts by weight of the ethylene/propylene randomcopolymer (EPR-1) prepared by the above polymerization was molded intoASTM specimens in the same manner as described in Example 1, to measurethe physical properties.

[1738] The results are set forth in Table 11. TABLE 11 Ex. 12 Comp. Ex.6 Propylene polymer (4) 50 50 Propylene polymer (11) 50 — Propylenepolymer (5) — 50 EPR-1 20 20 MFR (g/10 min) 12 15 FM (kg/cm²) 13,00013,000 IZ (23° C.) (kg · cm/cm) 28 12 EL (%) 430 180 HDT (load: 4.6 kg)(° C.) 97 105

Example 13

[1739] A propylene polymer composition consisting of 50 parts by weightof the propylene polymer (7), 50 parts by weight of the propylenepolymer (8), 10 parts by weight of the ethylene/propylene randomcopolymer (EPR-1) and 10 parts by weight of the ethylene polymer (PE-1)prepared by the above polymerization was molded into ASTM specimens inthe same manner as described in Example 1, to measure the physicalproperties.

[1740] The results are set forth in Table 12.

Example 14

[1741] A propylene polymer composition consisting of 50 parts by weightof the propylene polymer (7), 50 parts by weight of the propylenepolymer (8), 10 parts by weight of the ethylene/propylene randomcopolymer (EPR-3) and 10 parts by weight of the ethylene polymer (PE-2)prepared by the above polymerization was molded into ASTM specimens inthe same manner as described in Example 1, to measure the physicalproperties.

[1742] The results are set forth in Table 12. TABLE 12 Ex. 13 Ex. 14Propylene polymer (7) 50 50 Propylene polymer (8) 50 50 EPR-1 15 — EPR-3— 15 PE-1 10 — PE-2 — 10 MFR (g/10 min) 9.7 9.5 FM (kg/cm²) 13,90013,800 IZ (23° C.) (kg · cm/cm) 35 37 EL (%) 440 480 HDT (load: 4.6 kg)(° C.) 105 10

Example 15

[1743] A propylene polymer composition consisting of 100 parts by weightof the propylene polymer (9) and 25 parts by weight of theethylene/propylene random copolymer (EPR-1) prepared by the abovepolymerization was molded into ASTM specimens in the same manner asdescribed in Example 1, to measure the physical properties.

[1744] The results are set forth in Table 13.

Example 16

[1745] A propylene polymer composition consisting of 100 parts by weightof the propylene polymer (9), 20 parts by weight of theethylene/propylene random copolymer (EPR-1), both prepared by the abovepolymerization, and 15 parts by weight of a filler (talc) was moldedinto ASTM specimens in the same manner as described in Example 1, tomeasure the physical properties.

[1746] The results are set forth in Table 13.

Example 17

[1747] A propylene polymer composition consisting of 100 parts by weightof the propylene polymer (9), 10 parts by weight of theethylene/propylene random copolymer (EPR-3), 10 parts by weight of theethylene/1-butene random copolymer (EBR-1), all prepared by the abovepolymerization, and 15 parts by weight of a filler (talc) was moldedinto ASTM specimens in the same manner as described in Example 1, tomeasure the physical properties.

[1748] The results are set forth in Table 13. TABLE 13 Ex. 15 Ex. 16 Ex.17 Propylene polymer (9) 100 100 100 EPR-1 25 20 10 EBR-1 — — 10 Filler(talc) — 15 15 MFR (g/10 min) 9.0 9.8 10.3 FM (kg/cm²) 11,800 15,80018,800 IZ (23° C.) (kg · cm/cm) 55 44 40 EL (%) 750 310 310 HDT (load:4.6 kg) (° C.) 96 125 125

Example 18

[1749] A propylene polymer composition consisting of 100 parts by weightof the propylene polymer (9), 10 parts by weight of theethylene/propylene random copolymer (EPR-3) and 10 parts by weight ofthe ethylene/propylene random copolymer (EPR-4) prepared by the abovepolymerization was molded into ASTM specimens in the same manner asdescribed in Example 1, to measure the physical properties.

[1750] The results are set forth in Table 14.

Example 19

[1751] A propylene polymer composition consisting of 100 parts by weightof the propylene polymer (9), 10 parts by weight of theethylene/propylene random copolymer (EPR-3) and 10 parts by weight ofthe ethylene/propylene random copolymer (EPR-5) prepared by the abovepolymerization was molded into ASTM specimens in the same manner asdescribed in Example 1, to measure the physical properties.

[1752] The results are set forth in Table 14.

Comparative Example 12

[1753] A propylene polymer composition consisting of 100 parts by weightof the propylene polymer (10) and 20 parts by weight of theethylene/propylene random copolymer (EPR-1) prepared by the abovepolymerization was molded into ASTM specimens in the same manner asdescribed in Example 1, to measure the physical properties.

[1754] The results are set forth in Table 14. TABLE 14 Ex. 18 Ex. 19Comp. Ex. 12 Propylene polymer (9) 100 100 — Propylene polymer (10) — —100 EPR-1 — — 20 EPR-3 10 10 — EPR-4 10 — — EPR-5 — 10 — MFR (g/10 min)10.2 10.1 10.4 FM (kg/cm²) 13,000 12,700 12,000 IZ (23° C.) (kg · cm/cm)38 35 20 EL (%) 540 560 250 HDT (load: 4.6 kg) (° C.) 102 100 95

Example 20

[1755] A propylene polymer composition consisting of 100 parts by weightof the propylene polymer (14) and 20 parts by weight of theethylene/propylene random copolymer (EPR-1) prepared by the abovepolymerization was molded into ASTM specimens in the same manner asdescribed in Example 1, to measure the physical properties.

[1756] The results are set forth in Table 15.

Comparative Example 13

[1757] The propylene polymer (14) prepared by the above polymerizationwas molded into ASTM specimens in the same manner as described inExample 1, to measure the physical properties.

[1758] The results are set forth in Table 15. TABLE 15 Ex. 20 Comp. Ex.13 Propylene polymer (14) 100 100 EPR-1 20 — MFR (g/10 min) 7.2 9.5 FM(kg/cm²) 5,600 7,700 IZ (23° C.) (kg · cm/cm) 46 4.6 EL (%) 540 480

Example 21

[1759] A propylene polymer composition consisting of 100 parts by weightof the propylene polymer (9), 15 parts by weight of theethylene/propylene random copolymer (EPR-1) and 10 parts by weight ofthe ethylene polymer (PE-1) prepared by the above polymerization wasmolded into ASTM specimens in the same manner as described in Example 1,to measure the physical properties.

[1760] The results are set forth in Table 16.

Example 22

[1761] A propylene polymer composition consisting of 100 parts by weightof the propylene polymer (9), 15 parts by weight of theethylene/propylene random copolymer (EPR-3) and 10 parts by weight ofthe ethylene polymer (PE-2) prepared by the above polymerization wasmolded into ASTM specimens in the same manner, as described in Example1, to measure the physical properties.

[1762] The results are set forth in Table 16. TABLE 16 Ex. 21 Ex. 22Propylene polymer (9) 100 100 EPR-1 15 — EPR-3 — 15 PE-1 10 — PE-2 — 10MFR (g/10 min) 10.5 10.1 FM (kg/cm²) 13,500 13,200 IZ (23° C.) (kg ·cm/cm) 38 40 EL (%) 480 500 HDT (load: 4.6 kg) (° C.) 101 99

Example 23

[1763] A propylene polymer composition consisting of 100 parts by weightof the propylene polymer (6) and 20 parts by weight of theethylene/propylene random copolymer (EPR-3) prepared by the abovepolymerization was molded into ASTM specimens in the same manner asdescribed in Example 1, to measure the physical properties.

[1764] The results are set forth in Table 17. TABLE 17 Ex. 23 Propylenepolymer (6) 100 EPR-3 20 MFR (g/10 min) 17 FM (kg/cm²) 13,600 IZ (23°C.) (kg · cm/cm) 18 EL (%) 340 HDT (load: 4.6 kg) (° C.) 95

1. A propylene polymer composition which is the product obtained by theprocess comprising: polymerizing propylene or copolymerizing propyleneand at least one olefin selected from the group consisting of ethyleneand α-olefins of 4 to 20 carbon atoms in the presence of an olefinpolymerization catalyst comprising (i) a transition metal compound (h)represented by the following formula:

wherein M¹ is zirconium; R¹ is an alkyl group of 2 to 6 carbon atoms; R²is an aryl group selected from the group consisting of phenyl, naphthyl,anthracenyl and phenanthryl, wherein the aryl group is unsubstituted orsubstituted with a halogen atom or a hydrocarbon group of 1 to 20 carbonatoms; X¹ and X² are each a hydrogen atom, a halogen atom, a hydrocarbongroup of 1 to 20 carbon atoms, a halogenated hydrocarbon group of 1 to20 carbon atoms, an oxygen-containing group or a sulfur-containinggroup; and Y is a divalent silicon-containing group selected from thegroup consisting of dialkylsilylene, alkylarylsilylene anddiarylsilylene; and (ii) at least one compound selected from the groupconsisting of an organoaluminum oxy-compound, and a compound whichreacts with the transition metal compound (h) to form an ion pair, toprepare a propylene homo- or co-polymer (A); polymerizing orcopolymerizing at least one monomer selected from the group consistingof olefins of 2 to 20 carbon atoms and polyenes of 5 to 20 carbon atomsin the presence of an olefin polymerization catalyst which may be thesame or different from the aforementioned olefin polymerization catalystto prepare an olefin elastomer (D) which contains constituent unitsderived from ethylene, propylene, butene or 4-methyl-1-pentene in anamount of less than 90% by mol, and has a glass transition temperature(Tg) of not higher than 10° C.; polymerizing one monomer selected fromthe group consisting of ethylene, butene and 4-methyl-1-pentene orcopolymerizing said one monomer with at least one additional monomerselected from the group consisting of olefins of 2 to 20 carbon atomsother than said one monomer and polyenes of 5 to 20 carbon atoms, in thepresence of an olefin polymerization catalyst which may be the same ordifferent from the aforementioned olefin polymerization catalyst toprepare an olefin elastomer (D) which constituent units derive fromethylene, propylene, butene or 4-methyl-1-pentene in an amount of lessthan 90% by mol, and has a glass transition temperature (Tg) of nothigher than 10° C.; polymerizing one monomer selected from the groupconsisting of ethylene, butene and 4-methyl-1-pentene or copolymerizingsaid one monomer with at least one additional monomer selected from thegroup consisting of olefins of 2 to 20 carbon atoms other than said onemonomer and polyenes of 5 to 20 carbon atoms, in the presence of anolefin polymerization catalyst which may be the same as or differentfrom the aforementioned olefin polymerization catalyst to prepare anolefin polymer (E) which contains constituent units derived from saidone monomer in an amount of not less than 90% by mol; and mixing 5 to95% by weight of the propylene homo- or co-polymer (A), not more than95% by weight of the olefin elastomer (D), and not more than 95% byweight of the olefin polymer (E).
 2. A propylene polymer compositionwhich is the product obtained by a multi-stage polymerization methodcomprising the steps of: polymerizing propylene or copolymerizingpropylene and at least one olefin selected from the group consisting ofethylene and α-olefins of 4 to 20 carbon atoms in the presence of anolefin polymerization catalyst comprising (i) a transition metalcompound (h) represented by the following formula:

wherein M is zirconium; R¹ is an alkyl group of 2 to 6 carbon atoms; R²is an aryl group selected from the group consisting of phenyl, naphthyl,anthracenyl and phenanthryl, wherein the aryl group is unsubstituted orsubstituted with a halogen atom or a hydrocarbon group of 1 to 20 carbonatoms; X¹ and X² are each a hydrogen atom, a halogen atom, a hydrocarbongroup of 1 to 20 carbon atoms, a halogenated hydrocarbon group of 1 to20 carbon atoms, an oxygen-containing group or a sulfur-containinggroup; and Y is a divalent silicon-containing group selected from thegroup consisting of dialkylsilylene, alkylarylsilylene anddiarylsilylene; and (ii) at least one compound selected from the groupconsisting of an organoaluminum oxy-compound, and a compound whichreacts with the transition metal compound (h) to form an ion pair toprepare a propylene homo- or co-polymer (A); polymerizing orcopolymerizing at least one monomer selected from the group consistingof olefins of 2 to 20 carbon atoms and polyenes of 5 to 20 carbon atomsin the presence of an olefin polymerization catalyst which may be thesame as or different from the aforementioned olefin polymerizationcatalyst to prepare olefin elastomer (D) which contains constituentunits derived from ethylene, propylene, butene or 4-methyl-1-pentene inan amount of less than 90% by mol, and has a glass transitiontemperature (Tg) of not higher than 10° C.; polymerizing one monomerselected from the group consisting of ethylene, butene and4-methyl-1-pentene or copolymerizing said one monomer with at least oneadditional monomer selected from the group consisting of olefin of 2 to20 carbon atoms other than said one monomer and polyenes of 5 to 20carbon atoms in the presence of an olefin polymerization catalyst whichmay be the same as or different from the aforementioned olefinpolymerization catalyst to prepare an olefin polymer (E) which containsconstituent units derived from said one monomer in an amount of not lessthan 90% by mol; and wherein the steps of preparing the propylene homo-or co-polymer (A), preparing the olefin elastomer (D) and preparing theolefin polymer (E) are conducted in an arbitrary order; and the amountof the propylene homo- or co-polymer (A) is 5 to 95% by weight, and theamount of the olefin elastomer (D) is not more than 95% by weight, andthe amount of the olefin polymer (E) is not more than 95% by weight. 3.A propylene polymer composition which is the product obtained by theprocess comprising: polymerizing propylene or copolymerizing propyleneand at least one olefin selected from the group consisting of ethyleneand α-olefins of 4 to 20 carbon atoms in the presence of an olefinpolymerization catalyst comprising (i) a transition metal compound (h)represented by the following formula:

wherein M is zirconium; R¹ is an alkyl group of 2 to 6 carbon atoms; R²is an aryl group selected from the group consisting of phenyl, naphthyl,anthracenyl and phenanthryl, wherein the aryl group is unsubstituted orsubstituted with a halogen atom or a hydrocarbon group of 1 to 20 carbonatoms; X¹ and X² are each a hydrogen atom, a halogen atom, a hydrocarbongroup of 1 to 20 carbon atoms, a halogenated hydrocarbon group of 1 to20 carbon atoms, an oxygen-containing group or a sulfur-containinggroup; and Y is a divalent silicon-containing group selected from thegroup consisting of dialkylsilylene, alkylarylsilylene ordiarylsilylene; and (ii) at least one compound selected from the groupconsisting of an organoaluminum oxy-compound, and a compound whichreacts with the transition metal compound (h) to form an ion pair, toprepare a propylene homo- or co-polymer (A); polymerizing propylene orcopolymerizing propylene and not more than 10% by mol of at least oneolefin selected from the group consisting of ethylene and α-olefins of 4to 20 carbon atoms in the presence of an olefin polymerization catalystcomprising a metallocene compound or an olefin polymerization catalystcomprising (d) a solid titanium catalyst component and (e) anorganometallic compound catalyst component to prepare a propylene homo-or co-polymer (A′) which contains constituent units derived frompropylene in an amount of not less than 90% by mol and is different fromthe propylene homo- or co-polymer (A), wherein, the ratio of theintrinsic viscosity (η_(A)) of the propylene homo- or co-polymer (A) andthe intrinsic viscosity (ηA′) of the propylene homo- or co-polymer (A′),measured in decalin at 135° C., ((ηA/(ηA′) or ((ηA′/(ηA) is in the rangeof 3 to 30; polymerizing or copolymerizing at least one monomer selectedfrom the group consisting of olefins of 2 to 20 carbon atoms andpolyenes of 5 to 20 carbon atoms in the presence of an olefinpolymerization catalyst which may be the same as or different from theaforementioned olefin polymerization catalyst to prepare an olefinelastomer (D)which contains constituent units derived from ethylene,propylene, butene or 4-methyl-1-pentene in an amount of less than 90% bymol, and has a glass transition temperature (Tg) of not higher than 10°C.; polymerizing one monomer selected from the group consisting ofethylene, butene and 4-methyl-1-pentene or copolymerizing said onemonomer with at least one additional monomer selected from the groupconsisting of olefins of 2 to 20 carbon atoms other than said monomerand polyenes of 5 to 20 carbon atoms in the presence of an olefinpolymerization catalyst, which may be the same as or different from theaforementioned olefin polymerization catalyst, to prepare an olefinpolymer (E) which contains constituent units derived from said onemonomer in an amount of not less than 90% by mol; and mixing 5 to 95% byweight of the propylene homo- or co-polymer (A), not more than 95% byweight of the propylene polymer (A), not more than 95% by weight of theolefin polymer (E).
 4. A propylene polymer composition which is theproduct obtained by a multi-stage polymerization method comprising thesteps of: polymerizing propylene or copolymerizing propylene and atleast one olefin selected from the group consisting of ethylene andα-olefins of 4 to 20 carbon atoms in the presence of an olefinpolymerization catalyst comprising (i) a transition metal compound (h)represented by the following formula:

wherein M is zirconium; R¹ is an alkyl group of 2 to 6 carbon atoms; R²is an aryl group selected from the group consisting of phenyl, naphthyl,anthracenyl and phenanthryl, wherein the aryl group is unsubstituted orsubstituted with a halogen atom or a hydrocarbon group of 1 to 20 carbonatoms; X¹ and X² are each a hydrogen atom, a halogen atom, a hydrocarbongroup of 1 to 20 carbon atoms, a halogenated hydrocarbon group of 1 to20 carbon atoms, an oxygen-containing group or a sulfur-containinggroup; and Y is a divalent silicon-containing group selected from thegroup consisting of dialkylsilylene, alkylarylsilylene ordiarylsilylene; and (ii) at least one compound selected from the groupconsisting of an organoaluminum oxy-compound, and a compound whichreacts with the transition metal compound (h) to form an ion pair, toprepare a propylene homo- or co-polymer (A); polymerizing propylene orcopolymerizing propylene and not more than 10% by mol of at least oneolefin selected from the group consisting of ethylene and α-olefins of 4to 20 carbon atoms in the presence of an olefin polymerization catalystcomprising a metallocene compound or an olefin polymerization catalystcomprising (d) a solid titanium catalyst component and (e) anorganometallic compound catalyst component to prepare a propylene homo-or co-polymer (A′) which contains constituent units derived frompropylene in an amount of not less than 90% by mol and is different fromthe propylene homo- or co-polymer (A), wherein, the ratio of theintrinsic viscosity (η_(A)) of the propylene homo- or co-polymer (A) andthe intrinsic viscosity (η_(A)) of the propylene homo- or co-polymer(A′), measured in decalin at 135° C., ((η_(A)/(η_(A)) or ((η_(A)/(η_(A))is in the range of 3 to 30; polymerizing or copolymerizing at least onemonomer selected from the group consisting of olefins of 2 to 20 carbonatoms and polyenes of 5 to 20 carbon atoms in the presence of an olefinpolymerization catalyst which may be the same as or different from theaforementioned olefin polymerization catalyst to prepare an olefinelastomer (D)which contains constituent units derived from ethylene,propylene, butene or 4-methyl-1-pentene in an amount of less than 90% bymol, and has a glass transition temperature (Tg) of not higher than 10°C.; polymerizing one monomer selected from the group consisting ofethylene, butene and 4-methyl-1-pentene or copolymerizing said onemonomer with at least one additional monomer selected from the groupconsisting of olefins of 2 to 20 carbon atoms other than said monomerand polyenes of 5 to 20 carbon atoms in the presence of an olefinpolymerization catalyst, which may be the same as or different from theaforementioned olefin polymerization catalyst, to prepare an olefinpolymer (E) which contains constituent units derived from said onemonomer in an amount of not less than 90% by mol; and wherein the stepsof preparing the propylene homo- or co-polymers (A) and (A′), preparingthe olefin elastomer (D) and preparing the olefin polymer (E) areconducted in an arbitrary order; and the amount of the propylene homo-or co-polymer (A) is 5 to 95% by weight, the amount of the propylenehomo- or co-polymer (A′) is not more than 95% by weight, the amount ofthe olefin elastomer (D) is not more than 95% by weight and the amountof the olefin polymer (E) is not more than 95% by weight.
 5. Thepropylene polymer composition as claimed in claim 1, wherein thetransition metal compound israc-dimethylsilyl-bis(2-ethyl-4-phenylindenyl)zirconium dichloride. 6.The propylene polymer composition as claimed in claim 2, wherein thetransition metal compound israc-dimethylsilyl-bis(2-ethyl-4-phenylindenyl)zirconium dichloride. 7.The propylene polymer composition as claimed in claim 3, wherein thetransition metal compound israc-dimethylsilyl-bis(2-ethyl-4-phenylindenyl)zirconium dichloride. 8.The propylene polymer composition as claimed in claim 4, wherein thetransition metal compound israc-dimethylsilyl-bis(2-ethyl-4-phenylindenyl)zirconium dichloride.
 9. Apropylene polymer composition which is the product obtained by theprocess comprising: polymerizing propylene or copolymerizing propyleneand at least one olefin selected from the group consisting of ethyleneand α-olefins of 4 to 20 carbon atoms in the presence of an olefinpolymerization catalyst comprising (i) a transition metal compound (h)represented by the following formula:

wherein M is zirconium; R¹ is an alkyl group of 2 to 6 carbon atoms; R²is an aryl group selected from the group consisting of phenyl, naphthyl,anthracenyl and phenanthryl, wherein the aryl group is unsubstituted orsubstituted with a halogen atom or a hydrocarbon group of 1 to 20 carbonatoms; X¹ and X² are each a hydrogen atom, a halogen atom, a hydrocarbongroup of 1 to 20 carbon atoms, a halogenated hydrocarbon group of 1 to20 carbon atoms, an oxygen-containing group or a sulfur-containinggroup; and Y is a divalent silicon-containing group selected from thegroup consisting of dialkylsilylene, alkylarylsilylene anddiarylsilylene; and (ii) at least one compound selected from the groupconsisting of an organoaluminum oxy-compound, and a compound whichreacts with the transition metal compound (h) to form an ion pair, toprepare a propylene homo- or co-polymer (A); polymerizing orcopolymerizing at least one monomer selected from the group consistingof olefins of 2 to 20 carbon atoms and polyenes of 5 to 20 carbon atomsin the presence of an olefin polymerization catalyst which may be thesame or different from the aforementioned olefin polymerization catalystto prepare an olefin elastomer (D) which contains constituent unitsderived from ethylene, propylene, butene or 4-methyl-1-pentene in anamount of less than 90% by mol; polymerizing one monomer selected fromthe group consisting of ethylene, butene and 4-methyl-1-pentene orcopolymerizing said one monomer with at least one additional monomerselected from the group consisting of olefins of 2 to 20 carbon atomsother than said one monomer and polyenes of 5 to 20 carbon atoms, in thepresence of an olefin polymerization catalyst which may be the same ordifferent from the aforementioned olefin polymerization catalyst toprepare an olefin elastomer (D) which constituent units derive fromethylene, propylene, butene or 4-methyl-1-pentene in an amount of lessthan 90% by mol; polymerizing one monomer selected from the groupconsisting of ethylene, butene and 4-methyl-1-pentene or copolymerizingsaid one monomer with at least one additional monomer selected from thegroup consisting of olefins of 2 to 20 carbon atoms other than said onemonomer and polyenes of 5 to 20 carbon atoms, in the presence of anolefin polymerization catalyst which may be the same as or differentfrom the aforementioned olefin polymerization catalyst to prepare anolefin polymer (E) which contains constituent units derived from saidone monomer in an amount of not less than 90% by mol; and mixing 5 to95% by weight of the propylene homo- or co-polymer (A), not more than95% by weight of the olefin elastomer (D), and not more than 95% byweight of the olefin polymer (E).
 10. A propylene polymer compositionwhich is the product obtained by a multi-stage polymerization methodcomprising the steps of: polymerizing propylene or copolymerizingpropylene and at least one olefin selected from the group consisting ofethylene and α-olefins of 4 to 20 carbon atoms in the presence of anolefin polymerization catalyst comprising (i) a transition metalcompound (h) represented by the following formula:

wherein M is zirconium; R¹ is an alkyl group of 2 to 6 carbon atoms; R²is an aryl group selected from the group consisting of phenyl, naphthyl,anthracenyl and phenanthryl, wherein the aryl group is unsubstituted orsubstituted with a halogen atom or a hydrocarbon group of 1 to 20 carbonatoms; X² and x² are each a hydrogen atom, a halogen atom, a hydrocarbongroup of 1 to 20 carbon atoms, a halogenated hydrocarbon group of 1 to20 carbon atoms, an oxygen-containing group or a sulfur-containinggroup; and Y is a divalent silicon-containing group selected from thegroup consisting of dialkylsilylene, alkylarylsilylene anddiarylsilylene; and (ii) at least one compound selected from the groupconsisting of an organoaluminum oxy-compound, and a compound whichreacts with the transition metal compound (h) to form an ion pair toprepare a propylene homo- or co-polymer (A); polymerizing orcopolymerizing at least one monomer selected from the group consistingof olefins of 2 to 20 carbon atoms and polyenes of 5 to 20 carbon atomsin the presence of an olefin polymerization catalyst which may be thesame as or different from the aforementioned olefin polymerizationcatalyst to prepare olefin elastomer (D) which contains constituentunits derived from ethylene, propylene, butene or 4-methyl-1-pentene inan amount of less than 90% by mol; polymerizing one monomer selectedfrom the group consisting of ethylene, butene and 4-methyl-1-pentene orcopolymerizing said one monomer with at least one additional monomerselected from the group consisting of olefin of 2 to 20 carbon atomsother than said one monomer and polyenes of 5 to 20 carbon atoms in thepresence of an olefin polymerization catalyst which may be the same asor different from the aforementioned olefin polymerization catalyst toprepare an olefin polymer (E) which contains constituent units derivedfrom said one monomer in an amount of not less than 90% by mol; andwherein the steps of preparing the propylene homo- or co-polymer (A),preparing the olefin elastomer (D) and preparing the olefin polymer (E)are conducted in an arbitrary order; and the amount of the propylenehomo- or co-polymer (A) is 5 to 95% by weight, and the amount of theolefin elastomer (D) is not more than 95% by weight, and the amount ofthe olefin polymer (E) is not more than 95% by weight.
 11. A propylenepolymer composition which is the product obtained by the processcomprising: polymerizing propylene or copolymerizing propylene and atleast one olefin selected from the group consisting of ethylene andα-olefins of 4 to 20 carbon atoms in the presence of an olefinpolymerization catalyst comprising (i) a transition metal compound (h)represented by the following formula:

wherein M is zirconium; R¹ is an alkyl group of 2 to 6 carbon atoms; R²is an aryl group selected from the group consisting of phenyl, naphthyl,anthracenyl and phenanthryl, wherein the aryl group is unsubstituted orsubstituted with a halogen atom or a hydrocarbon group of 1 to 20 carbonatoms; X¹ and X² are each a hydrogen atom, a halogen atom, a hydrocarbongroup of 1 to 20 carbon atoms, a halogenated hydrocarbon group of 1 to20 carbon atoms, an oxygen-containing group or a sulfur-containinggroup; and Y is a divalent silicon-containing group selected from thegroup consisting of dialkylsilylene, alkylarylsilylene ordiarylsilylene; and (ii) at least one compound selected from the groupconsisting of an organoaluminum oxy-compound, and a compound whichreacts with the transition metal compound (h) to form an ion pair, toprepare a propylene homo- or co-polymer (A); polymerizing propylene orcopolymerizing propylene and not more than 10% by mol of at least oneolefin selected from the group consisting of ethylene and α-olefins of 4to 20 carbon atoms in the presence of an olefin polymerization catalystcomprising a metallocene compound or an olefin polymerization catalystcomprising (d) a solid titanium catalyst component and (e) anorganometallic compound catalyst component to prepare a propylene homo-or co-polymer (A′) which contains constituent units derived frompropylene in an amount of not less than 90% by mol and is different fromthe propylene homo- or co-polymer (A), wherein, the ratio of theintrinsic viscosity (η_(A)) of the propylene homo- or co-polymer (A) andthe intrinsic viscosity (ηA′) of the propylene homo- or co-polymer (A′),measured in decalin at 135° C., ((ηA/(ηA′) or ((ηA′/(ηA) is in the rangeof 3 to 30; polymerizing or copolymerizing at least one monomer selectedfrom the group consisting of olefins of 2 to 20 carbon atoms andpolyenes of 5 to 20 carbon atoms in the presence of an olefinpolymerization catalyst which may be the same as or different from theaforementioned olefin polymerization catalyst to prepare an olefinelastomer (D)which contains constituent units derived from ethylene,propylene, butene or 4-methyl-1-pentene in an amount of less than 90% bymol; polymerizing one monomer selected from the group consisting ofethylene, butene and 4-methyl-1-pentene or copolymerizing said onemonomer with at least one additional monomer selected from the groupconsisting of olefins of 2 to 20 carbon atoms other than said monomerand polyenes of 5 to 20 carbon atoms in the presence of an olefinpolymerization catalyst, which may be the same as or different from theaforementioned olefin polymerization catalyst, to prepare an olefinpolymer (E) which contains constituent units derived from said onemonomer in an amount of not less than 90% by mol; and mixing 5 to 95% byweight of the propylene homo- or co-polymer (A), not more than 95% byweight of the propylene polymer (A), not more than 95% by weight of theolefin polymer (E).
 12. A propylene polymer composition which is theproduct obtained by a multi-stage polymerization method comprising thesteps of: polymerizing propylene or copolymerizing propylene and atleast one olefin selected from the group consisting of ethylene andα-olefins of 4 to 20 carbon atoms in the presence of an olefinpolymerization catalyst comprising (i) a transition metal compound (h)represented by the following formula:

wherein M is zirconium; R¹ is an alkyl group of 2 to 6 carbon atoms; R²is an aryl group selected from the group consisting of phenyl, naphthyl,anthracenyl and phenanthryl, wherein the aryl group is unsubstituted orsubstituted with a halogen atom or a hydrocarbon group of 1 to 20 carbonatoms; X¹ and X² are each a hydrogen atom, a halogen atom, a hydrocarbongroup of 1 to 20 carbon atoms, a halogenated hydrocarbon group of 1 to20 carbon atoms, an oxygen-containing group or a sulfur-containinggroup; and Y is a divalent silicon-containing group selected from thegroup consisting of dialkylsilylene, alkylarylsilylene ordiarylsilylene; and (ii) at least one compound selected from the groupconsisting of an organoaluminum oxy-compound, and a compound whichreacts with the transition metal compound (h) to form an ion pair, toprepare a propylene homo- or co-polymer (A); polymerizing propylene orcopolymerizing propylene and not more than 10% by mol of at least oneolefin selected from the group consisting of ethylene and α-olefins of 4to 20 carbon atoms in the presence of an olefin polymerization catalystcomprising a metallocene compound or an olefin polymerization catalystcomprising (d) a solid titanium catalyst component and (e) anorganometallic compound catalyst component to prepare a propylene homo-or co-polymer (A′) which contains constituent units derived frompropylene in an amount of not less than 90% by mol and is different fromthe propylene homo- or co-polymer (A), wherein, the ratio of theintrinsic viscosity (η_(A)) of the propylene homo- or co-polymer (A) andthe intrinsic viscosity (η_(A)) of the propylene homo- or co-polymer(A′), measured in decalin at 135° C., ((η_(A)/(η_(A)) or ((η_(A)/(η_(A))is in the range of 3 to 30; polymerizing or copolymerizing at least onemonomer selected from the group consisting of olefins of 2 to 20 carbonatoms and polyenes of 5 to 20 carbon atoms in the presence of an olefinpolymerization catalyst which may be the same as or different from theaforementioned olefin polymerization catalyst to prepare an olefinelastomer (D)which contains constituent units derived from ethylene,propylene, butene or 4-methyl-1-pentene in an amount of less than 90% bymol; polymerizing one monomer selected from the group consisting ofethylene, butene and 4-methyl-1-pentene or copolymerizing said onemonomer with at least one additional monomer selected from the groupconsisting of olefins of 2 to 20 carbon atoms other than said monomerand polyenes of 5 to 20 carbon atoms in the presence of an olefinpolymerization catalyst, which may be the same as or different from theaforementioned olefin polymerization catalyst, to prepare an olefinpolymer (E) which contains constituent units derived from said onemonomer in an amount of not less than 90% by mol; and wherein the stepsof preparing the propylene homo- or co-polymers (A) and (A′), preparingthe olefin elastomer (D) and preparing the olefin polymer (E) areconducted in an arbitrary order; and the amount of the propylene homo-or co-polymer (A) is 5 to 95% by weight, the amount of the propylenehomo- or co-polymer (A′) is not more than 95% by weight, the amount ofthe olefin elastomer (D) is not more than 95% by weight and the amountof the olefin polymer (E) is not more than 95% by weight.